WHO PAHs Heavy Metal 1988

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343

ENVIRONMENTAL HEALTH
8 8 EM

32

Heavy Metal and PAH


Compounds from Municipal
Incinerators

i":-: ORGRGANIZATION
•{'** ilice for ,r.uropc
^
ENVIRONMENTAL HEALTH SERIES

1. Health Hazards from Nitrates in Drinking-Water: Report on


a WHO Meeting

2. Effects of Occupational Factors on Reproduction: Report on


a WHO Meeting

3. Neurobehavioural Methods in Occupational and Environmental


Health: Extended Abstracts from the Second International
Symposium

4. Reference Methods for Measuring Airborne MMMF

5. Chronic Effects of Organic Solvents on the Central Nervous


System and Diagnostic Criteria: Report on a Joint WHO/Nor-
dic Council of Ministers Working Group

6. Neurobehavioural Methods in Occupational and Environmental


Health: Reports from the Second International Symposium

7. Meeting Reports: Institutional Catering and Food Inspection

8. Treatment and Discharge of Industrial Wastewater in the


Mediterranean Area: Report on a WHO Meeting

9. Assessment of Noise Impact on the Urban Environment: A


Study on Noise Prediction Models

10. Environmental Toxicology and Ecotoxicology: Proceedings of


the Third International Course

11. Public Health Response to Acute Poisonings - Poison Control


Programmes: Report on a Joint Working Group

12. Occupational Health as a Component of Primary Health Care:


Report on a WHO Meeting

13. Indoor Air Quality: Radon and Formaldehyde: Report on a


WHO Meeting

14. Environmental Aspects of the Control of Legionellosis:


Report on a WHO Meeting

15. Health and Safety Component of Environmental Impact Assess-


ment: Report on a WHO Meeting
16. Health Impact of Low Indoor Temperatures: Report on a WHO
Meeting

17. PCDD and PCDF Emissions from Incinerators for Municipal


Sewage Sludge and Solid Waste: Evaluation of Human Exposure
Report on a WHO Meeting

18. Development of Environmental Health Manpower

19. Occupational Profiles of Environmental Health Personnel

20. Trace Elements in Human Health and Disease: Extended Ab-


stracts from the Second Nordic Symposium, 17-21 August 1987

21. Drinking-Water Quality and Health-Related Risks

22. Organophosphorus Pesticides: An Epidemiological Study.


Part 1. Meeting Report on Evaluation of the Pilot Phase of
the Study. Part 2. Core Protocol for the Study

23. PCBs,PCDDs and PCDFs: Prevention and Control of Accidental


and Environmental Exposures

24. Health Hazards from Radiocaesium Following the Chernobyl


Nuclear Accident: Report on a WHO Meeting

25. Nuclear Accidents and Epidemiology. Reports on two


meetings: Epidemiology Related to the Chernobyl Nuclear
Accident; Appropriate Methodologies for Studying Possible
Long—term Effects of Radiation on Individuals Exposed in a
Nuclear Accident

26. Trace Elements in Human Health and Disease: Symposium


Report from the Second Nordic Symposium, 17-21 August 1987

27. Drinking-Water Guidelines for Selected Herbicides: Report


on a WHO Meeting

28. Prevention of Acute Chemical Poisonings: High-Risk Circum-


stances: Report on a Joint WHO/IPCS/CEC Meeting

29. Assessment of Health Risks in Infants Associated with Ex-


posure to PCBs, PCDDs and PCDFs in Breast Milk

30. Eutrophication of Lakes and Reservoirs in Warm Climates

31. Guidelines for Healthy Housing


EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS
FROM MUNICIPAL SOLID WASTE INCINERATORS:
CONTROL TECHNOLOGY AND HEALTH EFFECTS

Report on a WHO meeting

Florence
12-16 October 1987

L'.EiV.XV, INTERNATIONAL REFERENCE \


• C E . IT..T P C S CO' ::.;jr^TY W A T E R S U P P L Y •
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•• . I

WORLD HEALTH ORGANIZATION


Regional Office for Europe
COPENHAGEN /
1988 .;• i ; [O
NOTE

This document has been prepared by the Regional Office for


Europe of the World Health Organization for governments of its
Member States in the Region. A limited number of copies are
available from the WHO Regional Office for Europe, Environment and
Health Service, Scherfigsvej 8, DK-2100 Copenhagen, Denmark.
The Environmental Health Series is intended to disseminate
rapid- ly information about activities of the WHO European
Environment and Health Service and has not received such detailed
editorial revision as WHO publications. Parties interested in
commenting, receiving more detailed information, or in collaborating
on specific activities are asked to contact the Director of the
Environment and Health Service, at the address given above.
The designations employed and the presentation of the material
in this volume do not imply the expression of any opinion whatsoever
on the part of the Secretariat of the World Health Organization con-
cerning the legal status of any country, territory, city or areas or
of its authorities, or concerning the delimitation of its frontiers
or boundaries. The mention of specific companies or of certain
manufacturers' products does not imply that they are endorsed or
recommended by the World Health Organization in preference to others
of a similar nature that are not mentioned. Errors and omissions
excepted, the names of proprietary products are distinguished by
initial capital letters.
For rights of reproduction or translation of this volume, in
part or in toto, application should be made to the address given
above. Such applications are welcome.
FOREWORD

In recent years, the incineration of municipal solid waste and


the resultant emission of toxic substances have generated worldwide
concern about possible adverse health effects. Such concern in
Italy prompted two meetings organized by the WHO Regional Office for
Europe at the request of Italian regional authorities in 1986 and
1987. The first meeting focused on the emissions of dioxins and
furans and the second meeting on the emissions of PAH and heavy
metal compounds.
This document reports on the deliberations, conclusions, and
recommendations of the second meeting held in October 1987 in
Florence to discuss control technology for and health effects from
incinerator emissions of heavy metal and PAH compounds. The meeting
was initiated and financed by the Regional Government of Tuscany, in
collaboration with the Government of Italy.
This report is aimed at the public and environmental health
authorities of the Tuscany Region, but it should be equally useful
to such authorities elsewhere as well as to professonals in this
area.

Michael J. Suess
Regional Officer for Environmental
Health Hazards
CONTENTS

Page

Foreword v

INTRODUCTION 1

WASTE AND INCINERATION 2

Types and characteristics of waste 3


MSW incineration technology 7
Control of incinerator emissions 9
Impact of incinerator operation on atmospheric emissions. . 12

DISCHARGE OF METALS AND PAH FROM INCINERATORS 15

Redistribution of elements during combustion 15


Atmospheric emissions and deposition 16
Incinerator ash 24
Government regulations 27

HEALTH-RELATED BACKGROUND 30

Human health concerns of cadmium, mercury, and lead . . . . 31


Health effects and critical populations 31
Human health concerns of PAH 32

SIGNIFICANCE OF MSW INCINERATOR EMISSIONS FOR HUMAN HEALTH . . 36

Technological aspects 36
Populations under consideration 37
Local health impact of cadmium 38
Local health impact of mercury 40
Local health impact of lead 40
Contribution of incinerator emissions to metal
exposure in the general population 41
Environmental release of metals from refuse
incineration compared with other sources 42
Contribution of incinerator emissions to PAH
exposure 47
Emissions of PAH from MSW incinerators compared with
other sources 49

VII
CONCLUSIONS AND RECOMMENDATIONS 50
Conclusions 50
Recommendations 52
REFERENCES 53
Annex 1: List of subgroups 6k
Annex 2: List of participants 65

vm
EHISSIONS OF HEAVY METAL AND PAH COHPOUNDS

INTRODUCTION

Emissions consisting mainly of dust, smoke, heavy metal


compounds, and noxious gases from municipal solid waste (MSW)
incinerators, sewage sludge incinerators, hazardous waste
incinerators, heating facilities, and thermal power plants have long
aroused concern. More recently, the potential danger of hazardous
organic compounds that may be present in emissions, such as
polycyclic aromatic hydrocarbons (PAH), has been recognized. The
high toxicity of some of these compounds has called into question
the safety of incinerating MSW. Answering these questions requires
a better understanding of the emission levels and potential adverse
public health effects of heavy metal and organic compounds, such as
PAH, emitted from MSW incinerators.
The WHO Regional Office for Europe organized a Working Group at
the request of the Regional Government of Tuscany, in collaboration
with the Government of Italy. The purpose of the meeting was to re-
view and discuss data and public health aspects related to the
emission of heavy metal and PAH compounds during incineration of
MSW. The Working Group's objective was to give national and local
health authorities, as well as other interested parties, guidance on
the public health significance of these emissions and, when possible
or necessary, to point out practicable approaches to minimize the
emissions and the related public health impacts. The meeting was
attended by 26 participants from 13 countries (Annex 2 ) .
Dr M. Piscator was elected Chairman, Mr A. Finkelstein and
Dr K. Kostial were elected Vice-Chairmen, and Mr C O . Velzy and
Dr A. Wadge each served as Co-Rapporteur. Dr M.J. Suess acted as
Scientific Secretary.
This meeting is the second on municipal waste incinerators or-
ganized by the WHO Regional Office for Europe in Italy. A working
group on dioxin and furan emissions met in Naples in 1986. The
report on the first meeting is available from the WHO Regional
Office for Europe [1].
The Working Group focused on the following major items:

- influence of the composition of the material being inciner-


ated, the conditions of the incineration process (temper-
ature, mixing, retention time of combustion products, oxy-
gen, and the operational aspects), and pollution control
technology and its operation on the quality and quantity of
emissions;

- environmental pathways of emitted heavy metal and PAH


compounds as related to human exposure;
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

- relative importance of MSW incineration compared with other


sources of human exposure to heavy metal and PAH compounds;

- public health significance of emissions of heavy metal and


PAH compounds during MSW incineration.

The Working Group broke into two subgroups (Annex 1 ) . Sub-


group 1 reviewed available data on emissions of heavy metal and PAH
compounds from MSW incinerators. This subgroup also considered and
evaluated aspects of design and operation to minimize incinerator
emissions. The results of these analyses and considerations were
organized into tables of expected emission concentrations from
incinerators of different types and with different operational
characteristics. Much of the descriptive text material on waste and
incineration in this report was extracted from the WHO Naples
meeting report [1].
Subgroup 2 summarized the potential human health aspects of
exposure to cadmium, mercury, lead, and PAH. It then evaluated the
relative contribution that emissions from incinerators may make to
the overall exposure of the general population to these pollutants.
As a starting point, subgroup 2 compared estimates of ground level
concentrations of emissions from MSW incinerators, developed from
measured stack emissions of these pollutants, with observed ambient
concentrations when available. Pollutant emissions were also com-
pared with inventories of regional or national emissions when avail-
able. These comparisons indicated different degrees of importance
for each pollutant of concern.

WASTE AND INCINERATION

MSW is a diverse and heterogeneous material generally con-


taining domestic and commercial waste. Domestic waste is solid waste
produced in the normal course of household activity or waste of a
similar character from institutions. Commercial waste is waste from
shops and offices, usually collected with domestic waste. MSW can
vary widely in physical composition (e.g. form, size, and consist-
ency) and chemical composition (e.g. carbon, hydrogen, oxygen,
nitrogen, chlorine, sulfur, metals, pesticides, plastics, and halo-
genated hydrocarbons). Industrial waste can introduce substantial
quantities of contaminants into the solid waste stream that would
otherwise exist only in trace amounts in MSW collected from resi-
dential and commercial areas. Only domestic and commercial solid
wastes are considered in this report.
A number of options exist for the processing and disposal of
MSW. In the past, some countries disposed of these materials at sea.
This method is now generally considered to be unsatisfactory because
of obvious adverse effects on, for example, marine life, and less
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

obvious effects, such as the introduction of contaminants into the


food chain. Alternate means of MSW disposal include deposition in
carefully designed, constructed, and operated landfills, composting
or separating component materials for recycling or reuse, or in-
cineration. All of these disposal options produce residuals that
must ultimately be disposed of in properly managed landfills. In
this report, only incineration is considered from a detailed pro-
cessing standpoint.
Incineration is defined in the WHO Glossary on solid waste [2]
as "the process of reducing combustible waste to an inert residue by
high temperature burning". This process has several outputs, such as
solid, liquid, and gaseous emissions, and heat energy. The primary
function of an incinerator is to reduce waste to an inert residue
with minimum adverse impact on the environment. Thermal efficiency,
while important, is secondary to this function. MSW incinerators are
usually classified according to their capacity, the nature of the
waste to be burned, the type of grate system used, and the method of
waste heat extraction, flue gas cooling, and gas cleaning. The
capacity of an incinerator in terms of quantity of waste processed
per unit of time is roughly inversely proportional to the heat value
of the waste.
Modern incineration plants reflect significant advances made in
solving the technical and practical difficulties of material hand-
ling and combustion control. In the early days of waste incineration
when air pollution regulations were undemanding or nonexistent,
relatively simple, fixed-grate plants operating on a single- or two-
shift basis were common. With increasingly stringent regulations to
control air pollution, more complex plants requiring continuous
operation have become the norm. Frequently, regulations and/or
requirements make small plants prohibitively expensive to operate.
In this report, the removal efficiencies and emission test
results from different installations are presented in terms of
"traditional" and "advanced" incinerators. Traditional incinerators
include all facilities incorporating normal combustion controls plus
dry particulate collection devices with an efficiency of approxi-
mately 95 to 97X. Advanced plants include facilities incorporating
modern combustion control systems and acid gas control scrubbing
equipment with a particulate control efficiency of 99X+.

Types and characteristics of waste

Two types of waste are considered in this report: as-collected


or as-received MSW and processed MSW.

As-received MSW

Some typical compositions of as-collected MSW can be calculated


(Table 1). In western Europe, waste composition varies over a wide
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

range. A typical analysis of MSW samples in western Europe and


United States is shown in Table 2.
Recent tests on MSW at two plants in the United States con-
ducted by the US Bureau of Standards [5] have shown average chlorine
contents ranging from 0.45 to 0.89% by mass of the total dry as-
received waste. Of the total chlorine, approximately 0.14 to 0.46%
by mass was from plastic materials, while approximately 0.31 to
0.43X by mass was from all other material. Thus, the variation in
chlorine from plastics was about 2.3 times the minimum level at
0.14X by mass, while the variation in chlorine from all other
material was about 0.4 times the minimum level at 0.311 by mass.
Therefore, the chlorine content in MSW probably depends greatly on
the total plastic content.

Processed MSW

Waste processing or separation technologies can affect the


chemical composition of MSW, which can vary widely and include or-

Table 1. Average composition of as-collected MSW

Type of waste Western Europe USA Middle East


city
X4 Range in X" X* X4

Organic 21.3 15-40 22.6 62.3


Paper 27.4 8-43 45.6 25.3
Textiles 3.5 1- 6 4.5 1.4
Plastics 3.1 3- 7 2.6 5.8
Glass 9.5 5-11 6.2 1.0
Metals 8.5 3- 8 9.1 2.8
Ash dust 19.8 2-60 7.6 NA
Miscellaneous 6.9 4 1.8 1.4

Total 100.0 100.0 100.0

" [3].
b
Personal communication from experts at the WHO meeting on
PCDD and PCDF Emissions from Incinerators for Municipal Sewage
Sludge and Solid Waste - Evaluation of Human Exposure, Naples, 17-21
March 1986.
NA = Not available.
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 2. Analysis of MSW

Type of analysis Weight by %*


Western United
Europe6 Statesc

Proximate analysis

Combustible 42.1 50.3


Water 31.0 25.2
Ash and inert material 26.9 24.5

Total 100.0 100.0

Ultimate (elemental) analysis


of combustibles

Carbon 51.1 50.9


Hydrogen 7.1 6.8
Oxygen 40.1 40.3
Nitrogen 1.2 1.0
Sulfur 0.5 0.4
Chlorine NA 0.6

Total 100.0 100.0

* Gross heat value, as fired = 9000 kJ/kg.


b
[3].
c
[4]; Domalski, E.S. et al., paper given at the 1986 National
Waste Processing Conference.
NA = Not available.

ganic and inorganic compounds. MSW can contain the following inor-
ganic compounds: cadmium, as a pigment, a stabilizer in plastics or
a surface coating, or in alloys and batteries; lead, in batteries,
lead-based paints, various metal items, and dusts; mercury, in bat-
teries, and in electrical and control equipment, and organomercuric
compounds in paper manufacturing; beryllium, in fluorescent light
bulbs; and inorganic metallic salts, in paper manufacturing [6].
Some organic compounds can be potentially troublesome: hexane,
toluene, and xylene in oil and acrylic paints, turpentines and other
solvents, and lithographic inks; methylene chloride, in paint
strippers and propellents for spray paint aerosol cans; formal-
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

dehyde, in particle board and plywood; dioxins, a contaminant in


pentachlorphenol wood preservatives; and various organic compounds,
in paper manufacturing.
Some of these substances, such as lead, mercury, and cadmium,
can contaminate the environment, regardless of the MSW disposal
method. Therefore, when developing a management plan for the dis-
posal of MSW, consideration should be given to collecting separately
some material containing these compounds, such as batteries, and
disposing of this material under tightly controlled conditions. In
other cases, consideration should be given to substituting less
hazardous materials. This approach can best be achieved at a
national or international level.
Trace organic compounds are widely distributed in the total
mass of MSW, and most of them can be destroyed in a properly de-
signed and operated waste combustion unit. However, some types of
waste processing, such as composting or materials recovery (e.g.
reclamation of paper fibre) may not destroy these substances [6].
Many countries have voluntary programmes of source separation,
including Italy, the United Kingdom, and the USA. Such programmes
have not had a significant impact on the composition of MSW. In
areas where bottles are returned and reused, as much as 50% of the
glass may be recycled [7]. However, as glass usually represents 10%
or less of MSW, the combustion process will be little affected.
Paper collection at the source is usually restricted to newspapers
and magazines. In countries with advanced separate collection
systems, up to 45% of the paper consumed may be recycled. This re-
duction may considerably lower the heat value of MSW.
Several programmes have been initiated to remove certain
potentially toxic substances from the solid waste stream prior to
incineration. In Zurich, Switzerland, mercury emissions from in-
cinerators were essentially the same before and after implementation
of a public education programme for removal of mercury-containing
batteries from the waste stream [8]. Sweden has a similar programme
for removal of batteries at source. While the effectiveness of the
programme to reduce incinerator emissions of mercury has not been
fully evaluated, results from the 2nd and 3rd quarters of 1987 (when
the programme started) indicate that approximately 50% of mercury
and 20% of cadmium in batteries were collected. The goal is to re-
cover 75% of the mercury in batteries (K. Hasselgren, Swedish
Association of Public Cleansing and Solid Waste Management, personal
communication, 1988).
Information is limited on the impact on emissions of removing
certain waste constituents from burning refuse-derived fuel (RDF).
Few plants use waste processing or material separation technologies.
In Italy, a very small proportion of plants (approximately 10%) use
mechanical processing for sorting metals, plastics, glass, or
organic matter (the last processed by composting for agricultural
use). Canada has only one mechanical processing system in oper-
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

ation; it uses shredding and magnetic metal separation. In the USA,


many RDF plants have been shut down [9].
Lorber [10] describes a testing programme investigating
emissions from combustion of as-received MSW and RDF. Emission tests
indicate that the concentration of hydrogen chloride, cadmium, and
lead in the untreated flue gas from the RDF combustion unit was in
the same range as that found in the flue gas of an MSW incinerator
before electrostatic precipitation and scrubbing [11]. These pollu-
tants were removed when the RDF was burned in a cement kiln where
the pollutants were fixed in the cement clinker.
In the United Kingdom, experiments are using mechanical sorting
in a rotary drum to produce a "cleaner" product to be used in RDF
production [12]. Preliminary processing results (Table 3) produced
160 tonnes of product (>40 ran) and 110 tonnes of reject material
(<40 mm). Most of the glass, approximately half of the putrescible
material, and about one third of the nonferrous metal were removed.
A significant portion of the lead and mercury (about two thirds and
one half, respectively) from nonmetallic sources was discharged to
the rejects (Table 4 ) . Rejection of heavy metals contained within
metallic items can only be inferred from the category data
(Table 3 ) ; a magnetic separation stage would be helpful in this
respect. Emissions have not been analysed for heavy metal compounds.
However, considering Lorber's results, one would expect to see
a major difference in heavy metal content in the stack emissions.
Boiler efficiency was calculated to increase from 68.3% when burning
raw waste to 73.2% when burning RDF. To the extent to which this
increase in boiler efficiency indicates improved combustion con-
ditions, it may also indicate lower emissions of organics, but no
test results are available to evaluate this theory.
Thus, careful consideration should be given to determining, in
detail, the trace chemical content of solid wastes before choosing
an overall solid waste management strategy.

MSW incineration technology

Waste combustion is a complex process. MSW is heated by contact


with hot combustion gases or preheated air and by radiation from the
furnace walls. The temperature range for drying is 50 to 150 °C.
At higher temperatures, volatile matter is formed by thermal decom-
position reactions. This volatile matter is generally combustible
and, after ignition, produces flames. The remaining material is
further degassed and burns much more slowly.
The combustion of MSW proceeds without supplementary fuel when
the heat value is at least 5000 kJ/kg. This occurs when the waste is
within the following general compositional limits: ash content,
<60%; moisture content, <50%; and combustible matter, >25%.
The complexity of the combustion of solids stems from the
nature of the decomposition and burning reactions and their
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 3. Analysis of RDF [12]

Material Feed Reject Product


(>40 mm) (<40 mm)
(% by weight)

Ferrous metals 6.4 41.0 99.0


Nonferrous metals 0.9 24.0 76.0
Glass 6.4 79.0 21.0
Putrescible material 20.8 30.0 50.0
Textiles 2.6 2.0 98.0
Paper and board 24.3 4.0 96.0
Plastics 7.3 5.0 95.0
Miscellaneous
Combustible 4.6 5.0 95.0
Noncombustible 4.0 73.0 27.0
Fines (<10 mm) 22.7 92.0 8.0

Total 100.0 41.0 59.0

association with heat transfer, air flow, and diffusion. In


most incinerators, combustion takes place while the solids
are supported on and conveyed by a grate. Since the early
1960s, most MSW incinerators have incorporated one of a
number of proprietary grate systems that allow a continuous
feed of unscreened waste into and movement through furnaces
with integral boiler facilities. The grate performs several
functions: providing support for the burning bed of refuse;
admitting und'erfire air through openings in the grate sur-
face; transporting the solid waste from feed mechanism to
ash quench; agitating the bed; and redistributing the
burning mass.
Combustion air is introduced as primary air and sec-
ondary air. Primary air passes through the grate and the
fuel bed and assists in burning the fuel and cooling the
grate. Secondary air is blown into the furnace through
nozzles above the fuel bed to promote mixing and complete
combustion of the burning gases. In some plants, tertiary
air is added to control the temperature of the flue gases
to required levels before discharge from the combustion
area.
During combustion, the heat value of the fuel is con-
verted into high-temperature flue gas and ashes, and into
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 4. RDF product analysis [12]

Analysis Feed Reject Product X of total


(>40 nan) (<40 mm) Reject Product

Gross calorific
value (MJ/kg) 9.2 6.62 11.0 29.6 70.4
Net calorific
value (MJ/kg) 7.91 5.57 9.53 28.9 71.1
Moisture content 31.4 32.1 31.0 41.7 58.3
(X by weight)
Ash content 30.5 42.8 21.9 57.6 42.4
(% by weight)
Volatiles (X by
weight) 31.6 14.4 43.7 18.4 81.6
C (X by weight) 28.8 28.7 29.0 40.8 59.2
H 2 (X by weight) 2.52 1.04 3.55 17.0 83.0
Oz (X by weight) 12.4 4.9 17.6 16.3 83.7
N (X by weight) 0.71 0.65 0.74 38.0 62.0
S (X by weight) 0.28 0.43 0.18 62.0 38.0
Cl (X by weight) 0.35 0.14 0.49 17.4 82.6
Pb (X by weight) 0.011 0.019 0.006 57.8 32.2
Cd (X by weight) 0.0012 0.0004 0.0017 16.4 83.6
Hg (X by weight)* 0.00004 0.00003 0.00004 41.0 59.0

a
Identifiable metal pieces were removed from samples prior
to chemical analysis. Hence metal content and distribution refer
only to nonmetallic sources.

heat losses through the furnace walls. With an estimate of heat


losses and the unburned carbon in the residue, the theoretical
combustion temperature can be calculated. This temperature may be
controlled by introducing varying quantities of excess air into the
furnace.
When waste with a low heat value is incinerated or when high
combustion temperatures are desirable, heat losses may be kept to a
minimum by adequate insulation of the furnace. The combustion tem-
perature may also be increased by preheating the combustion air or
by predrying or heating the waste products.

Control of incinerator emissions

Gas cleaning is required to reduce the level of pollutants in


EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

the raw flue gases (Table 5 ) . Electrostatic precipitators (ESP) are


the most commonly used gas cleaning device for particulate emission
control in municipal incinerators as they can be designed to achieve
very high collection efficiencies (99% or higher) and their oper-
ating costs are moderate. However, the investment cost and volu-
metric space required are high.
Fabric filters can operate at high efficiency even in the sub-
micron particle size range. Until recently, they were not widely
used in solid waste incineration plants because of their relatively
high investment and operating costs, and limited life at high
temperatures. However, with the increasing emphasis of regulatory
agencies on acid gas control and an apparent trend to lower parti-
culate emission levels, baghouses, usually in conjunction with ad-
dition of lime, and lower flue gas temperatures are being used more
widely with municipal waste incinerators in the USA.
Wet collectors were initially used to control acid gas. Various
semi wet and dry methods of cleaning flue gases have also been used.
These methods of gas treatment, based on the injection of slurried
or powdered lime, limestone, or dolomite, eliminate a large fraction
of the acid gases from the flue gas by adsorption and absorption,
followed by chemical conversion. Because the reactivity of these
lime materials is rather low, a multiple of the stoichiometric
quantity is normally required to obtain a satisfactory cleaning
effect. High removal efficiencies can be achieved for hydrogen
chloride, but reduction of sulfur dioxide and sulfur trioxide is

Table 5. Typical composition of raw flue gases (vet basis,


NTP*)[3]

Substance Amount

H20 10 - 18 % by volume
CO* 6 - 12 % by volume
O2 7 - 14 % by volume
CO < 0.1 % by volume
Dust 2 - 15 g/m3
Cl" 250 - 2000 mg/m3 (as HC1)
F" 0.5 - 5 mg/m3 (as HF)
S0 2 + SO3 100 - 1000 mg/m3 (mainly S0 2 )
NO + NOz 100 - 400 mg/m3 (largely as NO)

NTP = normal temperature and pressure.

10
EMISSIONS OF HEAVY HETAL AND PAH COMPOUNDS

only partial. However, slaked lime is highly reactive and stoichio-


metric ratios of 1.2 to 1.7 have been used for 97-991 of hydrogen
chloride removal and 60-901 reduction of sulfur dioxide, depending
on operating conditions and particulate collector. Lime injection
into a scrubber/fabric filter system has removal efficiencies of
90-991 for hydrogen chloride and 70-9OX for sulfur dicxide, provided
that the flue gas temperature, certain equipment design features,
and stoichiometric ratio for lime addition are suitable.
Test results for MSW incinerators equipped with the conventional
two-field ESP have shown a wide range of particulate emissions,
varying from 50 to 300 mg/Nm3 (0.07 to 0.13 grains per dry stan-
dard cubic foot (gr/dscf)). The three- and four-field ESP (see
Table 6) can achieve emissions of 20 to 75 mg/Nm1 (0.009 to 0.03
gr/dscf). An emission level below 20 mg/Nm3 (0.009 gr/dscf) is
technically possible and ha6 been demonstrated at Zurich (J.T.
MbHer, personal communication, 1986) where lime addition was retro-
fitted on a plant with an existing two-field ESP.
The scrubber/fabric filter control systems have also been shown
(see Table 6) to be capable of operating at a particulate emission
level of 20 mg/Nm3 (0.009 gr/dscf) and lower. The material
selected for the filter bags can have an important effect on filter-
ing efficiency and the emission level thus achieved. In general,
test results for the scrubber/fabric filter indicate lower parti-
culate emissions than those for ESP on MSW incinerators, though ESP
have not normally been designed to meet emission levels as low as
those specified for fabric filter installations. In Europe, ESP fol-
lowing spray drying absorbers have been tested at particulate
emission levels of 1 to 8 mg/Nm' (0.00045-0.0036 gr/dscf). The
reliability and overall economics of the various control processes
must be considered when making a selection of equipment to meet
these very low emission control requirements.
Because the condensation point for most metals, such as com-
pounds of lead, cadmium, chromium, and zinc, is above 300 °C, the
removal efficiency of such metals depends highly on the removal
efficiency of the particulate control system used. Some heavy metal
compounds, particularly chlorides, have condensation points below
300 "C. For such compounds, particulate collection temperatures
will be a factor in collection efficiency. High removal (over 99%)
has been observed for most metals for highly efficient (over 991)
particulate removal systems operating at appropriate temperatures
[13].
Traditional incineration facilities have relatively inefficient
particulate control equipment and emissions of metals may be rela-
tively high in such facilities (Table 7).
Mercury, a very volatile metal, exists in vapour phase at
temperatures as low as 20 to 50 °C. Several studies have sug-
gested that both sufficient cooling of the flue gas (typically below
140 °C, based on test results) and a highly efficient particulate

11
EMISSIONS OF HEAVY HETAL AND PAH COMPOUNDS

removal system to remove the particles on which the mercury has been
actively absorbed [14,15] (H. Vogg et al., paper presented at Fifth
International Recycling Congress, 1986) are required to achieve high
mercury removal. High mercury removal has also been obtained using
the scrubber/fabric filter and semidry/ESP systems, provided that
the flue gas is adequately cooled [13]. Properly operated wet
scrubbers are also capable of considerably reducing mercury
emissions (Goepfert, Reimer and Partners, unpublished report, 1986).
Data on emissions of PAH and other chlorinated organic com-
pounds are limited. Most sampling programmes for PCDD/PCDF, which
have been fairly extensive, have unfortunately neglected to analyse
for these compounds. The scrubber/fabric filter technology generally
demonstrated removal rates of 80-99X for these compounds [13].

Impact of incinerator operation on atmospheric emissions

An advanced incinerator is designed to achieve 991 conversion of


organic matter to carbon dioxide [16]. This objective is achieved by
providing adequate residence time, postcombustion temperature, and
turbulent mixing. When this objective is achieved, the concentration

L
Table 6. Participate emissions froa HSU incinerators

Plant Dry filterable material


(at 12X COz)
gr/dscf mg/Nm3

G (1983); ESP 0.0321 72


T (1984); DS.FF 0.0120 27
M (1984); DS.EP 0.0104 23
W (1985); DS.FF 0.0040 9
P (1985); ESP 0.0163 37
T (1986); ESP 0.0070 16
M (1986); DS.FF 0.0070 16

1
per Engineers, 1984,
Unpublished reports: Cooper 1984, :1985; Bahn
et al., 1986; Velzy, 1986, 1987).
DS = Dry or semidry scrubber (lime addition).
ESP a Electrostatic precipitator.
FF * Fabric filter (bag house).
gr/dscf a Grains per dry standard cubic foot.

12
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

level of carbon monoxide remains consistently below 0.1% by volume.


Generally, levels of 125 mg/Nm1 (100 ppm) and less are achievable
in advanced design plants with modern combustion control systems.
Combustion may be incomplete when the incinerator is im-
properly operated in the following ways:

- inadequate mixing of the feed material so that large quan-


tities of material with extremely high or low heat value
enter the furnace;

Table 7. Removal efficiencies foe certain metals from flue gases


from MSW incinerators

Equipment Particulate- PAH Vapour-


bound bound
(Cd, Pb) (Hg)
Removal efficiency (%)

Traditional

High eff. ESP1 Cd 95-99+ NA


Pb 95-99+ 20%

Advanced

1. Scrubber + Cd 98-99++ 80-90% (at 120-


ESP2 1A0 °C)
(Semidry) Pb 98-99++
2. Scrubber + FF3 Cd 99++ 99 85-95% (at 140 °C)
(Dry) Pb 99++ 99 Much uncertainty
3. Wet4 Cd 99+ 70•-90%"
Pb 99+

ESP = Electrostatic precipitator. FF = Fabric filter (baghouse).


NA = Not applicable.
1
Data from measurements in Europe and North America.
2
J.T. Mbller, personal communication, 1986 and 1987.
3
R. Bergstrom, personal communication, 1986.
4
A. Nottrodt, personal communication.
* Dry endproduct 60-75%
b
Liquid effluent 80-95%

13
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

- operation at excessively low temperatures (some regulatory


agencies require the use of auxiliary burners when the tem-
perature at the exit from the combustion chamber drops below
800 °C);

- quenching of the flames caused by improper distribution of


secondary air;

- gross overloading of the plant.

Incomplete combustion can be detected by monitoring the flue


gas composition. Conventional combustion gas measurements include
carbon monoxide, total hydrocarbons, and oxygen or carbon dioxide.
Both carbon monoxide and total hydrocarbons have been of interest as
potential surrogates to indicate incomplete combustion or periods of
poor combustion. Under these poor combustion conditions, carbon
monoxide levels of several thousand mg/Nra3 have been observed and
total hydrocarbon levels have risen from a typical 1.25 to
6.25 mg/Nm3 (1-5 ppra) to 125 mg/Nm3 (100 ppm) and more.
Poor combustion conditions in incinerators can lead to local
oxygen-deficient conditions, resulting in the emission of hazardous
organic compounds. PAH, for example, are formed during fuel-rich
combustion as a consequence of free radical reactions in the high-
temperature flame zone. In addition, in the presence of water-cooled
surfaces, such as found in oil-fired home-heating furnaces, a high
fraction of the polycyclic compounds is oxygenated. Similar free
radical reactions probably take place in fuel-rich zones of inciner-
ator flames, yielding PAH, oxygenated compounds (e.g. phenols), and,
in the presence of chlorine, some PCDD and PCDF.
The amount of heavy metal compounds, other than those with low
vaporization such as mercury, discharged from an MSW incinerator is
largely a function of the amount of fly ash discharged. The amount
of ash carried with the flue gases from a burning refuse bed in-
creases with increasing underfire air rate and with bed agitation.
For this reason, starved or controlled air incinerators with low
underfire air flow rates tend to have lower particulate emissions
from the furnace than conventional mass-burn units. In addition, the
particle size of the inorganic content of the MSW will influence the
amount of ash carried from the combustion chamber.
High-efficiency particulate control devices can effectively
reduce the atmospheric emission of most heavy metal compounds. As
the efficiency of particulate control improves, metal emissions
generally decrease and, in most cases, decrease significantly. Even
though ample evidence from tests [17,18] (W. Dannecker, personal
communication, 1983) indicates that heavy metals tend to concentrate
on the finer particles, evidence also suggests that more than 99%
metal removal from flue gases can be achieved by using high effi-
ciency (99%) particulate control devices (Cooper Engineers, un-

14
EHISSIOHS OF HEAVY HETAL AND PAH COHPOUNDS

published report, 1985; Hahn et al., paper given at National Waste


Processing Conference, 1986).

DISCHARGE OF METALS AND PAH FROM INCINERATORS

Organic materials composed entirely of carbon, hydrogen, and


oxygen will produce water and carbon dioxide as the final products
of complete combustion in the presence of oxygen. However, MSW in-
cludes many compounds or elements in addition to the three elements
noted above. Therefore, discharges to the environment emanating from
the burning of MSW include substances resulting directly from com-
bustion and other substances present in the bed of solid waste. Dis-
charges may be in the form of stack gas and particulate emissions,
bottom ash from the furnace grates, and fly ash from the removal of
particulates in the flue gases.
Metals are not produced by the incineration process but rather
are changed, concentrated or redistributed among the various process
effluents. This is in contrast to PAH, which are largely generated
as a consequence of incomplete combustion.

Redistribution of elements during combustion

The distribution of elements between bottom ash and ash carried


to the air pollution control device depends upon the design and
operation of the incinerator and the composition of the feed. The
distribution of elements among the different components of refuse
also strongly influences the fate of the elements. For example,
titanium dioxide, a pigment in paper products, has a particle size
of about 0.2 um and will tend to be carried off by the flue gases
passing through the refuse bed, whereas titanium dioxide in glass
will end up in the bottom ash. About 10X of the inorganic content of
the waste will be entrained from burning refuse beds to form fly ash
particles [19]. The remainder will end up in the residue.
Volatile elements and their compounds, usually present in trace
amounts in the feed, will vaporize from the refuse and condense in
the cooler portions of a furnace either as an ultrafine aerosol (<
1 um in diameter) or on the surface of fly ash particles. A large
fraction of highly volatile elements in the feed, such as mercury,
will be volatilized and emitted to the atmosphere in vapour form
unless special preventive measures are taken. Some elements may be
converted to more volatile chemical forms during combustion. For
instance, the relatively high chlorine content of MSW results in an
adequate supply of hydrogen chloride to form substantial quantities
of volatile metal chlorides [17] as well as chlorinated organic com-
pounds .
PAH concentrations in MSW incineration residues are relatively
uniform (Table 8 ) . However, the metals increase in concentration

15
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

from bottom ash, to boiler/economizer ash, to precipitator or fly


ash. Greenberg et al. [17] suggest that trace element enrichment on
fine particles is primarily due to a volatilization-condensation
mechanism similar to that proposed by Natusch et al. [20] for
coal-fired power plants. The proportionately greater surface area of
fine fly ash particles is expected to result in an enrichment of
the volatile trace elements on these particles. However, Wadge et
al. [18] suggests that the elevated levels of certain trace elements
in incinerator fly ash may result not from a
volatilization-condensation mechanism but, in part at least, from
the loss of organic fraction in the furnace. This would leave an
inorganic residue enriched in trace elements.
Using the information in Tables 7 and 8, the distribution of
selected metals and PAH in incinerator residues can be calculated
(Table 9). The concentrations of refractory elements such as iron,
carbon monoxide and titanium will be higher in the bottom ash.

Atmospheric emissions and deposition

Cadmium, lead, and mercury

A review of data on cadmium, lead, and mercury indicated that


emissions were significant (Tables 10-12). The emission levels or
toxicities of other metals were so low that they were considered to
be of minor importance.

Table 8. Concentrations of PAH, certain metals, chlorine, and sul-


fur in MSV-incinerated residues1

Subs tance Bottom Boiler/economizer Precipitator


ash ash ash

PAH (ug/g) 0.1-0.5 0.03-0.2 0.2-0.5


Cd (ug/g) 2.0-7.5* 115-350 250-1100*
Pb (ug/g) 750-6000* 5000-16000 5000-26000*
Hg (ug/g) 0.01-1.0* 1-8 5-70*
Cl (mg/g) 3-6* ND 40-80*
S (mg/g) 2-4* ND 20-40*

Personal communications: P.H. Brunner, A. Nottrodt, J.T.


Moller.
* [19,21].
ND = Not detected.

16
Table 9. Emission factors and distribution (X of input) for selected metals
and PAH [22]

Compound Bottom ash Boiler ash Fly and Fly ash from stack
g/t of
waste
% g/t of
waste
boiler ash
g/t of
waste
Tradi-
tional
«as cleaning
Advanced 8
t/»
g/t of
g/t of waste %
waste

HEAVY METAL AND PAH COMPOUNDS


Cadmium 0.4-2 10-40 0.1-4 3-30 55-80 0.4-9 0.1-0.25 1-15
Lead 200-2000 55-80 5-200 50-800 20-45 0.6-300 0.06-5 1-5
Mercury 0.1-0.3 2-6 0.001-0.06 0.05-2 15-35 0.6-10 0.2-1.3 60-85
PAHa 20-150 45-12 0.03-2.0 1.5-14 4-1 20-1000 50-80

a
Distribution in percentage is not based on PAH concentrations in MSW
input.
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 10. Emission data on cadmium from stacks

Traditional dry collection Advanced acid gas control


95% +/- efficiency scrubber (dry or wet/dry)
99% +• efficiency

Canada* Canada*

0.6-1.0 mg/Nm3 - 12% C 0 2 SA N.D.-0.6 ug/Nm3 - 8% 0 2


0.02-1.0 mg/Nm3 - 12% C 0 2 MB w/scrubber and FF
MB w/ESP

France" France"

0.06-0.1 mg/Nm3 - 7% C 0 2 0.03 mg/Nm3 - 7% C 0 2 (wet)


(wet) MB MB w/ESP and scrubber
1-1.5 mg/Nm3 - 7% C 0 2 0.001-0.003 mg/Nm3 - 7% 0 2
(wet) MB (wet) MB, DS and FF

Italy0 Italy/

0.83 mg/Nm3 - 10% 0 2 (wet) MB 0.02 mg/Nm3 - 10% 0 2 (wet) MB

Switzerland" Switzerland"

0.1-2.0 mg/Nm3 - 7% C 0 2 0.01 mg/Nm3 - 11% 0 2

United Kingdom* Federal Republic of Germany11

0.16-0.45 mg/Nm3 - 10% C 0 2 00.2 mg/Nm3 - 11% 0 2


(dry) MB MB w/SDA and ESP
0.04 mg/Nm3 - 12% 0 2
United States' MB w/wet scrubber

0.2-0.5 mg/Nm3 - 12% C 0 2 (dry) MB


0.2-1.2 mg/Nm3 - 7% 0 2 (dry) SA
0.5-0.7 mg/Nm3 - 7% 0 2 (dry) RDF w/ESP

DS = Dry scrubber. ESP = Electrostatic precipitator. FF = Fabric


filter. MB = Mass burn. ND = Nondetectable. RDF = Refuse-
derived fuel. SA = Starved air. SDA = Spray drier-absorber.
[13,26,27]. Dimitrov, paper given at Third National Seminar
of the Air Quality Agency, 1987. [28]. [29]. [30].
[31]. [32]. J.T. Moller, personal communication,
1986. J.T. Moller, personal communication, 1987.

18
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 11. Emission data on lead from stacks

Traditional dry collection Advanced acid gas control


95% +/- efficiency scrubber (dry or wet/dry)
99% + efficiency

Canada* Canada*

0.6-2.5 mg/Nm3 - 12% C 0 2 0.002-0.006 mg/Nm3 - 8% 0 2


MB w/ESP MB w/scrubber and FF
8.0-15.0 mg/Nm3 - 12% C0 2 SA

France" France"

34-49 mg/Nm3 - 7% C0 2 0.055-0.07 mg/Nm3 - 7% C0 2


(wet) MB (wet) MB, DS and FF
1.3-1.9 mg/Nm3 - 7% C 0 2 0.78 mg/Nm3 - 7% C0 2 (wet)
(wet) MB w/ESP MB w/ESP and scrubber

Italy" Italyc

19 mg/Nm3 - 10% 0 2 (wet) MB 0.54 mg/Nra3 - 10% 0 2 (wet)

Switzerland*1 Switzerland"

1-18 mg/Nm3 - 7% C0 2 0.38 mg/Nm3 - 11% 0 2 MB w/SDA


and ESP

United Kingdomf Federal Republic of Germany8

2.4-10.7 mg/Nm3 - 10% C0 2 0.6 mg/Nm3 - 12% 0 2 MB w/wet


(dry) MB scrubber; 0.01 mg/Nm3 - 11% 0 2
MB w/SDA and ESP

United States"

0.15-22.0 mg/Nm3 - 7% 0 2 (dry) SA


1.5-1.8 mg/Nm3 - 7% 0 2 (dry) RDF w/ESP

DS = Dry scrubber. FF = Fabric filter. MB = Mass burn. RDF =


Refuse-derived fuel. SA = Starved air. SDA = Spray drier-absorber.
* [13,26,27]. Dimitrov, paper given at Third National Seminar
of the Air Quality Agency, 1987. " [28]. c [29]. [301.
f 3
° J.T. MSller, personal communication, 1986. [31]. J.T.
Moller, personal communication, 1987. h [32].

19
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 12. Emission data on mercury from stacks

Traditional dry collection Advanced acid gas control


95% +/- efficiency scrubber (dry or wet/dry)
99% + efficiency

Canada* Canada*

0.7-0.85 mg/Nm3 - 12% C0 2 0.01-0.6 mg/Nm3 - 8% 0 2


MB w/ESP MB w/scrubber
0.5-0.7 mg/Nm3 - 12% C0 2 SA

Federal Republic of Germany" Federal Republic of Germany*

0.42-0.62 mg/Nm3 - 11% 0 2 0.07-0.08 mg/Nm3 - 12% 0 2


MB w/SDA and ESP MB w/wet scrubber

France0 Francec

0.5-0.66 mg/Nm3 - 7% C0 2 (wet) <0.06 mg/Nm3 - 7% C0 2 (wet)


MB w/ESP and scrubber
<0.22 mg/Nm3 - 7% C0 2
(wet) MB, DS and FF

Italy" Italy"

0.1 mg/Nm3 - 10% 0 2 (wet) MB 0.01 mg/Nm3 - 10% 0 2


(wet) MB

Switzerland* Switzerland f

0.3-1.5 mg/Nra3 - 7% C0 2 0.035 rag/Nm3 - 11% 0 2


MB w/SDA and ESP

United Kingdom"

0.5-0.6 mg/Nm3 - 10% C0 2


(dry) MB

20
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 12. (cont'd)

USAh USA"
1.2-2.2 mg/Nm3 - 7% 0 2 0.028 mg/Nm3 - 12% C0 2
(dry) MB w/ESP (dry) MB w/wet/dry
0.4-0.6 mg/Nm3 - 7% 02 scrubber and FF
(dry) RDF w/ESP
2.0 mg/Nm3 - 71 0 2 (dry) MB
2.2 mg/Nm3 - 12% C0 2 (dry) SA

DS = Dry scrubber. ESP = Electrostatic precipitator.


FF = Fabric filter. MB = Mass burn.
RDF = Refuse-derived fuel. SA = Starved air.
SDA = Spray drier-adsorber.
a
[13,26,27]. " J.T. Moller, personal communication, 1987.
Dimitrov, paper given at Third National Seminar of the Air
Quality Agency, 1987. c [28]. d [29]. * [30]. f Moller,
personal communication, 1986. ° [31]. h [32].

21
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Cadmium emissions range between 0.06 and 2.0 mg/Nm3 for


traditional plants and 0.001 and 0.04 mg/Nm3 for advanced plants
(Table 10). The lowest specific test result was 0.00004 mg/Nm3 for
an advanced plant [23]. However, as the specific conditions of this
plant operation and its design features are unknown, this result
should not be included in the range of anticipated test results.
Test results for lead ranged between 0.2 and 50 mg/Nm3 for tradi-
tional plants and 0.01 and 0.8 mg/Nm3 for advanced plants (Table
11). Test results for mercury ranged between 0.1 and 2.2 mg/Nm3
for traditional plants and 0.03 and 0.2 mg/Nm3 for advanced plants
(Table 12). Results for advanced plants for mercury removal depend
largely on temperature and technology.
Table 13 gives ranges of stack emission rates of cadmium,
lead, and mercury from incinerators in Europe, Canada, and the USA.
To calculate the increase in ambient air concentration given in
Table 13, a dilution factor of 5 x 10" s was used. This factor is
lower than the one used in the dioxin report of the WHO meeting in
Naples [II. This value corresponds to the value based on the model
of the TA-Luft [24]. To calculate the dilution factor for deposition
rates, two different values have been chosen:

cadmium and lead (2 x 10" z ug/m 2 /d)


ug/m

mercury and PAH (2 x 10* 3 ug/m 2 /d)


na/m
ug/m

The value of 2 x 10" z has been derived from preliminary re-


search on the dry and wet deposition of cadmium and lead in the
vicinity of MSW incinerators [25]. The value of 2 x 10' 3 refers to
the model of the German TA-Luft 1986 for industrial incinerators.
In conclusion, the results indicate that traditional MSW in-
cinerators may have a significant impact on the ambient air concen-
tration as well as on the deposition rates of cadmium and lead. In
contrast, the contributions from advanced MSW incinerators are in
the range of the background levels or even less.
Table 9 summarizes the element emission factors (in grams per
tonne of input MSW) and distributions (in percent of input MSW) for
the data available for analysis at this meeting. The distribution
of the elements depends on the element properties as well as on the
design and operation of the incinerator and gas cleaning system, and
the composition of the MSW.

PAH

A wide range of PAH has been identified in the various effluents


arising from MSW incineration [33,34]. A number of studies have as-
sessed PAH in various parts of incinerators. However, there is a

22
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 13. Emission, ground-level concentration, and deposition


rates for selected metals and PAH

Compound Stack Calculated Rural Calculated Background


emissions increase in background increase in deposition
(mg/NmJ) ambient air ambient air deposition rates
concentration (ng/Nm3) rates (wet (ug/m2/d)
(ground level) and dry) 5
(ng/Nm3)* (ug/m2/d)

Cd (2) 0.06-2 3-80 <l-5 1-40 0.5-2


(3) 0.001-0.04 0.05-2 0.02-0.8

Pb (2) 0.2-50 8-3000 50-300 3-1000 40


(3) 0.01-0.8 0.5-40 0.2-20

Hg (2) 0.1-2.2 5-10 1-4 0.2-4 1-<1


(3) 0.03-0.2 2-10 0.02-1

PAH (4) 0.003-0.2(5) 0.1-<0.10(5) 0.006-0.4 -

* Dilution factor for ambient a i r concentration, 5 x 10" s (see t e x t ) .


(1) Dilution factor for deposition of Cd, Pb (2 x 10" 2 ), Hg and PAH (2 x
3
10" ) (see t e x t ) .
(2) Traditional incinerator.
(3) Advanced incinerator.
(4) No differentiation between traditional and advanced except as noted.
(5) Large value stands for small-scale incinerator (<500 kg/h), which may
produce high air concentration due to low stack height.

23
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

lack of consistency in the individual PAH reported and the methods


of sampling and analysis used. Consequently, data are insufficient
to derive good mass balance determinations that relate the amount of
material entering, synthesized in, and leaving the incinerator
system.
In a well-run plant, PAH in the refuse feed material are un-
likely to persist through the combustion process. More probably,
PAH in the various effluent streams result from incomplete com-
bustion of ordinary non-PAH carbonaceous material or high-temper-
ature free radical mechanisms [35,36].
The most important emission pathways of PAH are via the flue
gases and the bottom ash, due to the significantly greater mass of
bottom ash compared to that of other plant residuals. PAH account
for less than 1% of the total organic carbon (TOC) in the products
of incineration.
Based on a review of test results, stack emissions were tabu-
lated for PAH and benzo(a)pyrene (BaP) (Table 14). Very little in-
formation is available that would allow a separate projection of PAH
emissions for "traditional" and "advanced" plants.
The contribution of incinerator emissions to background ambient
air concentrations and deposition rates of PAH can be estimated
(Table 13) using dilution factors of 5 x 1O'S and 2 x 10' 3 ,
respectively, based on the model of the German TA-Luft [24].

Incinerator ash

During incineration, 98 to 99% of the organic matter of MSW is


converted to carbon dioxide and other volatile compounds, resulting
in a mass reduction of 65 to 75%. Depending on the composition of
the MSW, about 200 to 300 kg of bottom ash is produced per tonne of
MSW. The volume of this bottom ash corresponds to about 10% of the
initial MSW volume. The amount of filter ash is approximately 10%
of the mass of the bottom ash, depending on the operating conditions
of the furnace and the gas cleaning system. Ash deposited in the
economizer and boiler will vary from 1.0 to 10.0 kg/t of initial
MSW. If dry or wet/dry acid gas control scrubber systems are used
for emission control, the mass of filter dust or combined fly ash
and chemical treatment additive (usually lime) will be increased by
25 to 150%.
As noted earlier, fly ash contains higher concentrations of
volatile metals compared with bottom ash (Table 8 ) . Precipitator
ash contains higher chloride and sulfur concentrations than bottom
ash (Table 8), which together with the smaller particle size and the
different chemical form of the element indicates a greater tendency
for metals to leach from the precipitator ash than from the bottom
ash. Experiments (P.H. Brunner & P. Baccini, paper given at Second
International Conference on New Frontiers for Hazardous Waste
Management, 1987; S.E. Sawell, unpublished report, 1987) [25] show a

24
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 14. Emission data on PAH from stacks

Data by country Technology

Total PAH

Canada*

0.005-0.02 mg/Nm3 Traditional MB


0.00002-0.00013 mg/Nm3 Advanced MB, w/scrubber and FF
0.007-0.012 mg/Nni Traditional MB (starved air)

Italy

0.0075-0.208 mg/Nm3 Traditional MB

Japan

0.04 mg/Nm3 Traditional MB (batch fed)


0.002 mg/Nm3 Traditional MB

Sweden"

0.001 mg/Nm3 Advanced

BaP only

Canada"

0.008-0.062 ug/Nm3 One traditional plant


O.0O0015-0.OO013 ug/Nm3 One advanced plant

Federal Republic of Germany

0.0005-0.005 ug/Nm3 Five traditional and advanced


plants

Italj

0.05-33* ug/Nm3 Four traditional and advanced


plants

25
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 14. (cont'd)

Japan

0.5-1.5" ug/Nm3 Two traditional plants

United States'

5.9-19 ug/Nm3 One traditional plant

* BaP and BeP combined data.


b
Assumed particulate emission rate of 100 mg/ra3.
MB = Mass burn. FF = Fabric filter.
m
[13,26,27] b [37] c [32]

high leachability at first water contact of the precipitator ash


(10% cadmium, 0.5% lead, 20% zinc with deionized water). With a high
content of calcium oxide, as used in acid gas treatment, the pH of
an aqueous suspension of filter ash rises to 9-10. At this pH, most
metals are present as insoluble hydroxides. However, a question re-
mains about the long-term behaviour of ash deposits. In a laboratory
study designed to examine long-term leaching patterns at landfill
sites, Wadge & Hutton [38] report a relatively rapid movement of
cadmium and lead from incinerator fly ash.
Several factors have the ability to change the mobility of
metals in an ash deposit: pH changes, complexing agents, and micro-
bial activity. At pH 3-4, 85% of the cadmium, 5% of the lead, and
50% of the zinc in ash are mobilized (Sawell, unpublished report,
1987) [25]. If lime or other products are added during gas purifi-
cation, the pH and the salt content change, which alters the
physicochemical behaviour of the filter residue (mobility of the
amphoteric elements). Thus, to ensure safe long-term behaviour in a
natural environment, further treatment of flue gas cleaning residues
may be required.
The content of organic matter in the filter residues is about
10 to 40 g/kg. Less than 1% of the compounds in this fraction has
been identified. Of those identified, the largest group consists of
chlorinated benzenes (approximately 1 ug/g), PAH (0.2-0.5 ug/g), and
chlorinated phenols (approximately 0.5 ug/g) [16]. The organic com-
pounds are tightly bound to particle surfaces and are not mobile in
an aqueous environment if organic solvents are absent. An exception
is chlorinated phenols, which may go into solution. Still unknown is
the extent to which carbon can be used by microbial activities, re-
ducing pH levels and changing the leaching characteristics of ash

26
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

deposits (P.H. Brunner & F. Baccini, paper given at Second Inter-


national Conference on New Frontiers for Hazardous Waste Management,
1987).
Research on disposal of MSW incinerator ash residues addresses
the following topics:

- concentration of the hazardous elements in the ash, in-


cluding controlled leaching of the metals at different pH;

- fixation of the metals in the residues by vitrification or


solidification (cementor silica-based) [39,40];

- destruction of carbonaceous residues by optimizing com-


bustion and reheating filter dust;

- leach tests to determine the long-term behaviour of residues


from MSW incineration in the natural environment;

- plant availability of metals in incinerator residues [41].

Government regulations

Canada, the USA, and most countries in Europe have regulations


covering emissions from MSW incinerators. Regulations normally
establish specific control levels for the emissions of, for example,
dust, carbon monoxide, oxides of nitrogen, heavy metal compounds,
and acid gases, together with stipulations for the method of
monitoring and enforcement.
Pollution control agencies consider a number of factors that
influence their decisions on how to control MSW incineration, in-
cluding the following ones:

Plant-related factors. Some countries, such as France, feel


that large plants should be more strictly controlled than small
ones. Similarly, plants within residential areas may have to be
regulated more carefully than those well removed from towns. Other
factors within this category would include the type of plant, local
topography, and prevailing meteorological conditions.

Pollutant-related factors. Pollution control decisions will


also depend upon the nature of the substances to be controlled.
Some, such as specific metal compounds, can be relatively easily
sampled and analysed directly. Others, such as PAH, are very costly
to determine as individual compounds within this entire group of
compounds. Even with metals, it is arguable whether those metals of
similar toxicity should be identified and controlled as a group, as
is the case in France, rather than establishing emission limitations
for individual metals as is generally the case ia the USA. Also,

27
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

while the total amount of a metal is generally determined in a test,


sometimes the species are of interest.

Pollution control options. Another choice to be made is


whether action should be taken to control the process using specific
control limits or by specifying the equipment technology to be used.
Control limits can be applied either at the source directly or
as ambient air quality standards at the point of maximum source im-
pingement on a receptor. When applied at the source, operators are
allowed to choose the technology to control their plant emissions,
provided that set control limits are met. These limits would
specify the ""»<"•"• quantities of a substance that could be emitted
by any emission route, whether it be to air, water, or land. In the
case of a metal, the control limit could relate directly to the pol-
lutant, as is the case in many countries. In the case of PAH, which
are difficult to measure as a total listing of all compounds, in-
direct indicators might have to be used as surrogates. These are
analytes (such as BaP), which are relatively easy to determine and
vary in concentration as the target species would. This approach
has some attractions, but the identification of suitable surrogates
is difficult and, in the case of PAH, would require further research
work.
In some cases, ambient air quality standards have been adopted:
for example, the Council of the European Communities Directive on
the limit value for lead in the air (OJ L 378, 31 December 1982).
This approach is useful when the pollutant is emitted from a large
number of small sources.
Specific control procedures are a commonly used alternative or
addition to setting control limits. The control equipment or tech-
nology that an operator should adopt is specified (i.e. best avail-
able control technology, BACT), bearing in mind that this should not
entail excessive costs. This approach is being adopted increasingly
by the Council of the European Communities. It is also somewhat
similar to the best practicable means (BPM) system used in the
United Kingdom.

When both the substances to be controlled and a well-defined


control technology can be identified, legally binding emission stan-
dards can be set, as many countries have with metals. But in the
case of PAH, the compounds most hazardous to health can probably not
be identified or a clear consensus arrived at as to the most cost-
effective control process. In these circumstances, recommendations
or guidelines are commonly used. While they are not legally
binding, they do indicate target values to be aimed at. This ap-
proach has proved useful for dioxin control in the past (i.e.
Sweden, Denmark, and Italy) and has encouraged interested parties to
identify the control issues and adopt appropriate control practices.

28
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

An implicit component of any control strategy is the need to


test whether a control requirement is being met; this is called com-
pliance testing. Broadly speaking, compliance testing has two main
approaches: monitoring to check emission levels and/or visits by
qualified inspection personnel.
The problems of monitoring emissions are considerable and
should not be underestimated. Neither should monitoring instrument-
ation and procedures be assumed to be sufficiently developed to be
accepted (as proof of plant malfunction) in a court of law.
Both regulatory pressures and technological advances have suc-
ceeded in transferring the environmentally harmful species from
stack emissions into the water effluents and residual ashes from MSW
incinerator. The legislation for the disposal of these effluents is
often less well developed than those for air pollution control and
may have to be modified in the future.

Regulations for MSW incinerator emissions

Many countries have national regulations for controlling


emissions of heavy metal compounds. These are constantly under
review, and listing the provisions of all the countries is im-
possible. Instead, the current proposals of the Commission of the
European Communities for new municipal waste incineration plants can
be given as an indication of possible regulations (Table 15). The
emission limit values in Table 15 are standardized at the following
conditions: temperature, 273 K; pressure, 101.3 KPa; and 11%
oxygen or 9% carbon dioxide (17% 0z in case of incineration plants
of a nominal capacity less than 1 tonne per hour).

Water and solid effluent provisions

Incinerators produce liquid effluents from ash quench tanks,


wet scrubbers, and other areas of water usage in the processing of
MSW. They also produce large quantities of residual ash for dis-
posal. Many countries have guidelines for the handling and disposal
of these effluents, but few have specific legislation that treats
solid and liquid effluents from MSW incinerators differently from
any other pollutant discharge. While a general discussion of water
treatment and solid waste disposal legislation is outside the scope
of this report, the specific problems of MSW ash handling have
prompted some governments, including France, the Federal Republic of
Germany, Sweden, Switzerland, and the USA, to consider legislation
calling for specific regulations for MSW incineration plants. These
proposals range from requirements to contain and treat wastewater
produced by MSW incineration prior to discharge, to requirements for
the segregation of ashes and the separate storage/disposal of fly
ash in special landfills.

29
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 15. Proposals of the Commission of the European Communities


for regulations foe MSW incinerator emissions

Pollutant Emission limit value1


(mg/Nm3)

Total dust 50 a
Heavy metals
Pb + Cr + Cu +Mn 5b
Ni + As l"
Cd + Hg 0.2b

Hydrochloric acid 50 a
Hydrofluoric acid 2b
Sulfur dioxide 300 b

1
These values do not apply to plants designed to burn refuse-
derived fuel and that use such fuels exclusively. The Commission
shall submit to the Council as soon as possible proposals for limit
values to be applied to these plants.
a
100 mg/Nm3 in case of incineration plants of a nominal
capacity less than 3 tonnes per hour.
b
These limits do not apply to incineration plants of a
nominal capacity less than 1 tonne per hour.

HEALTH-RELATED BACKGROUND

Major episodes of ill-health have been reported among popu-


lations acutely and chronically exposed to cadmium, lead, and mer-
cury arising from non-occupational sources other than MSW inciner-
ators [42-44]. Epidemiological studies have not been conducted in
the vicinity of MSW incinerators, but considerable amounts of cad-
mium and mercury are emitted from these facilities [30,45,46] and
lead is a major constituent of the metals in MSW [47]. For these
reasons, the metals of prime concern with respect to emissions from
MSW incinerators are cadmium, lead, and mercury.
This section summarizes the environmental pathways, metabolism,
toxicity, and human health effects of these three metals. Compre-
hensive reviews of their health effects are available [42,48-51].
The relative significance of metal and PAH emissions from MSW in-
cinerators compared with other high-temperature combustion and in-
dustrial processes is considered later.

30
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Human health concerns of cadmium, mercury, and lead

Exposure pathways

Generally, dietary intake is the major route of exposure for


the three metals. In the case of lead, inhalation is also an im-
portant source of exposure in urban-dwelling populations [51]. In-
fants may also ingest considerable quantities of lead by inadver-
tently consuming dusts or deliberately ingesting lead-rich paint or
soil [52,53]. Tobacco smoking can be an important source of cadmium
intake [54]. Methylmercury is the chemical species of mercury of
importance in environmental exposure, and, in the general popu-
lation, the major (>90%) source of this is fish consumption [55].
The three metals differ greatly in the percentage that is ab-
sorbed across the gastrointestinal tract. Methylmercury is absorbed
efficiently (approximately 95%) while the fractional absorption of
cadmium is only about 5%. This latter value increases considerably
in cases of iron deficiencies [56]. Lead absorption is often re-
ported to be about 10% in adults, but a higher value (approxi-
mately 50%) is often assumed in children [57,58].

Metabolism

Once absorbed, the three metals display characteristic tissue


distributions. Cadmium selectively accumulates in the kidney and
liver where it binds to the protein metallothionein [42]. In con-
trast, methylmercury is initially distributed throughout the body,
readily crossing the blood-brain barrier, although the kidneys re-
tain the highest tissue concentration [59]. Most of the lead (ap-
proximately 90%) is stored in the skeleton, but the liver and kidney
also contain relatively high concentrations. An important feature of
lead and methylmercury is that both easily cross the placental
barrier; this is particularly efficient for methylmercury. The pla-
cental barrier is more efficient for cadmium; the median blood cad-
mium of neonates was about 50% lower than in mothers [60].

Health effects and critical populations

Lead may affect two endpoints: the haematological system and


the central nervous system. The haematological effects arise at the
beginning and final steps of haem synthesis. Interference in the
last stage results in the accumulation of protoporphyrin in the
blood, which may occur at blood lead concentrations of about 15
ug/100 ml; that is, at concentrations regarded as "normal". At
higher levels of lead exposure, anaemia can develop. The haemato-
logical effects of lead are reversible.
Of potentially greater concern is the reported association
between certain neurobehavioural effects and lead exposure in ur-

31
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

ban-dwelling children [61]. Decreases in measurements of intelli-


gence and behaviour have been found in children from the general
population subjected to commonly occurring levels of lead exposure.
These effects are widely believed to reflect the greater suscepti-
bility of the fetus and child to lead resulting from greater sensi-
tivity of the developing central nervous system and higher intake
and uptake of the metal as compared with adults.
Methyltnercury intoxication is also characterized by effects on
the central nervous system, the major areas affected being associ-
ated with the sensory, visual, and auditory functions as well as
those concerned with coordination [55]. The developing nervous
system of the fetus is more sensitive than that of the adult, and
prenatal exposure can subsequently result in neurotoxic effects in
the infant in the absence of effects in the mother. Populations with
heavy fish consumption have been identified as being exposed to ele-
vated levels of methylmercury, which is enriched to a high degree in
the aquatic food chain [55].
The kidney is the critical organ of intoxication after long-
term exposure to cadmium [42]. Increased urinary levels of B 2 -
microglobulin (S2M), retinol-binding protein (RBP), and
N-acetyl-B-D-glucosaraidase (NAG) appear to be the most sensitive
parameters of early changes in tubular function. The concentrations
of BzM in serum and albumin in urine appear the most sensitive
parameters of changes in glomerular function. However, these forms
of proteinuria are not specific to cadmium [62-64]. Nevertheless,
measurement of BzM is being increasingly adopted to monitor for
the early effects of cadmium exposure.

Human health concerns of PAH

Environmental data and exposure pathways

About 500 PAH have been detected in air (Pott, address before
the Federal Council of Environment, Berlin (West), 1983), but re-
ports of ambient air levels of PAH dating from the 1950s to about
1970 are limited only to BaP only. These data are not necessarily
comparable with more recent reports because many different sampling
procedures and analytical methods have been used. The natural back-
ground level of BaP is determined by the production of PAH in vege-
tation [65] . PAH could be detected even in borings out of 140-m
depth more than 100 000 years old [66]. Compared with the anthro-
pogenic load, the natural background level of PAH in air amounts to
not more than 1%.
The annual average of BaP concentrations in urban European
locations often exceeded 100 ng/m3 in the 1960s [67], while more
recent measurements in the Federal Republic of Germany and USA in-
dicate that levels are now mostly below 10 ng/m3 [67,68].

32
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Daily intake of BaP by inhalation of polluted ambient air con-


taining a relatively high concentration of 50 ng/m 3 , which is
similar to the levels found in the vicinity of coke oven plants
[69], is estimated at 400 ng BaP [51]. However, the BaP intake in
clean rural areas and cities where adequate smoke control has been
achieved may be only a few percent of this or less. Tobacco smoke
will add to the inhalation of PAH. Modern "low-tar" cigarettes
deliver 10 ng BaP [70], while Grimmer et al. [71] measured 22
ng/m3 of BaP in a room heavily polluted with cigarette smoke.
Concentrations of BaP in drinking water range from 0.1 to 23
ng/1 [72]. The possible sources of PAH in foodstuffs are varied and
extremely widespread. Curing smokes, contaminated soils, polluted
air and water, modes of cooking, food additives, food processing,
and endogenous sources have been investigated. Some 100 PAH have
been identified and numerous reviews are available [72-74]. BaP con-
centrations up to 50 ug/kg were measured in broiled and smoked food
[73], and BaP concentrations ranging from 2 to 540 ug/kg have been
reported in shellfish [75]. A person in the German Democratic
Republic is estimated to ingest 24 to 85 mg BaP during his or her
lifetime (70 years) [72]. The daily intake of BaP from food is
estimated to range from 0.16 to 3.0 ug in the USA [76].
For most people, oral intake of PAH is considerably greater
than the amount inhaled. Much attention has been given to the role
played by inhalation of PAH in causing respiratory tumours, but the
evidence is not clear whether, and to what extent, ingested PAH may
be implicated in respiratory or other tumours.

Uptake and metabolism

PAH are highly lipid-soluble and are absorbed across the lungs,
gut, and skin of mammals. As most of the PAH in the ambient air are
attached to fine particles, the potential health effects of PAH
after inhalation depends on the deposition rate in the respiratory
tract, residence time in the lung, the dissolution rate of PAH from
the particles, and the chemical structure. Furthermore, the overall
composition of the particulate matter (i.e. the ratio of the mass of
the carbonaceous core to the mass of the attached organic material)
is a factor in determining the biological half-life of the particle-
related PAH in the lungs. Particles that consist mainly of organic
material, such as coal tar aerosols, will be eliminated from the
lungs almost completely within 24 hours. In contrast, the lung
clearance half-life of soot particles, which consist mainly of car-
bonaceous material, such as diesel soot, is relatively long [77].
PAH associated with the latter particle types may exert a stronger
carcinogenic effect in the lungs because their residence time is
longer.
In general, PAH metabolism consists of a series of oxidation
steps catalysed by monoxygenases and epoxide hydrase. Metabolites

33
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

include epoxide intermediates, dihydrodiols, phenols, quinones, and


their combination. After being metabolized to dihydrodiols, some of
the epoxides can be further oxidized to diol epoxides. These latter
compounds are generally thought to be the ultimate carcinogens [72].
Oxidized metabolites of PAH are later conjugated with glucu-
ronic acid, glutathione and sulfonic acid, forming polar metabolites
that are more easily excreted from the body [78,79].

Toxicity data and biological effects in laboratory animals

Toxic effects of PAH have not been studied as well as their


oncogenic effects. Longer-term oral exposures to PAH have resulted
in various systemic effects in animals, but overt signs of toxicity
are not usually produced until the dose is sufficiently high to pro-
duce tumours [72].
Although embryotoxic, teratogenic, and immunosuppressive ef-
fects have been observed in some assays, PAH are not acutely toxic
compounds.
Several PAH and some of their metabolites have been shown to be
mutagenic in mammalian cells and bacterial assays [72,78-80].
The ability of individual PAH to produce neoplasia has been
intensively researched for some 50 years, particularly on induction
of skin tumours in rodents by topical application of PAH. The car-
cinogenicity of selected PAH in rodents by different routes of ad-
ministration has been recently summarized [81].
BaP-induced tumours usually develop at the site of application.
For example, rats fed BaP develop forestomach tumours [82] while
intraperitoneal infection leads to hepatic tumours when pheno-
barbital, a promoter, is added to the diet [83], and inhalation
induces respiratory tract tumours [84]. Respiratory tract car-
cinogenicity of BaP is enhanced when this compound is coadministered
with particulates, such as ferric oxide, or is absorbed to the ad-
ministered particles [85].
Many substituted PAH, such as nitro-, methyl- and oxygenated
PAH, are also likely in combustion products. Many of these compounds
are mutagenic in in vitro tests, and some have been reviewed for
evidence of human carcinogenicity [72].

Human health effects

Data summarized by IARC [49] demonstrate carcinogenicity to


humans from industrial exposures to mixtures containing PAH. These
occupational exposures include aluminium production, coal gasifi-
cation, coke production, and iron and steel founding. Bitumens,
coal tars and derived products, shale oils, and soots have also been
evaluated for their human health effects (skin cancer) [86]. A de-
tailed evaluation of the carcinogenicity of PAH in coke oven
emissions has been published [87].

34
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Epidemiological studies of these workplaces provide sufficient


evidence of the role of inhaled PAH in inducing lung cancer [88-92].
However, levels of PAH in these workplaces were very high, often
exceeding 10 ug/m3 BaP [49,93,94], which is several orders of mag-
nitude greater than in ambient air. In addition to high PAH levels,
other carcinogenic gases and metals were present in the occupational
settings studied. For example, coke oven emissions may contain other
carcinogenic agents, including arsenic, chromium, nickel(VI),
2-naphthylamine, and benzene.
Cigarette smoking is strongly and consistently associated with
cancer at several sites, including the lung, larynx, oral cavity,
oesophagus, bladder, and kidney [95,96]. Thirty-four PAH, some of
which are recognized carcinogens, have been identified in mainstream
and sidestream cigarette smoke [72].
Little is known about the possible implications for human
health of PAH in food and water, and the role of PAH in toxic end-
points other than carcinogenicity has not been well studied. There-
fore, on the basis of available experimental results, the carcino-
genic potential of PAH is considered the most significant health
effect for the general population.

Characterization of potential human health risk from PAH

A major difficulty in hazard assessment of PAH is that the data


for compounds other than BaP are very limited, and that from most
emissions, such as those from municipal waste combustion, the full
range of PAH has not been analysed. The hazard assessment of this
diverse but related group of components would benefit from a model
of biological effects compared with those of a well-studied com-
pound, as has been done for dioxins. To this end, several attempts
have been made to compare carcinogenic activity of various PAH with
that of BaP [81]. At present, however, such a comparative ranking
seems prudent only for the most general of classification.
Because several PAH are carcinogenic [49,87] and data for BaP
are most extensive, BaP is normally used as an index of the carcino-
genic potential of all PAH in a sample. However, PAH profiles
detected in different types of industrial emission and workplace air
can differ widely.
Several approaches have been taken to provide quantitative
estimates of potential human risk from PAH exposure. WHO [51] cal-
culated a unit risk of 9 x 10" s cases of cancer for a lifetime
exposure to 1 ng/m3 BaP. This upper bound of estimates is derived
by application of the linearized multistage procedure to data for
lung tumour incidence among coke oven workers [81,91] and using a
reported value of 0.71% BaP in benzene-soluble coke oven emissions
[97]. This risk assessment implies that about 9 per 100 000 exposed
people may die from cancer of the respiratory tract as a result of
spending a lifetime in ambient air containing an average level of

35
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

1 ng/m3 BaP in a mixture with all the other PAH and related sub-
stances of coke oven emissions.

SIGNIFICANCE OF MSW INCINERATOR EMISSIONS FOR HUMAN HEALTH


Emissions from MSW incinerators, in common with many high-tem-
perature combustion and other industrial processes, contain a wide
range of inorganic and organic compounds, including metals and PAH
[31,32,34,45]. When assessing potential health hazards, emissions of
metals and PAH from incinerator plants must be considered in con-
junction with pollution from other pertinent sources in the area. In
Czechoslovakia, for example, coal combustion has been identified as
an important source of this type of emissions [98-100].
This section considers the significance of MSW incinerator
emissions for human health Occupational hazards are not considered
here, but workers in incinerator plants will be exposed to dust and
fumes containing metals and PAH [101]. The problems encountered will
be similar to those in other industrial plants where furnaces are
operated.

Technological aspects

MSW incinerators initially included less efficient air pol-


lution control equipment than required by most current regulations.
Thus, the emissions of pollutants were high, as can be seen from
examples cited in Tables 10-12 and IU. The impact of such emissions
on the environment can be assessed only in rough terms, using data
on (a) the likely concentrations of toxic chemicals in the vicinity
of the plants, resulting from modelling computations, (b) actual
measurements of the concentrations in the air close to incinerators
as compared with the background levels, and (c) measurements of
toxic chemicals in soil and vegetation near incinerators.
In cases (b) and (c), measurements at various distances from
the plant are helpful in evaluating the real impact, that is, the
increase above the local background level.
Although such data on the impact of traditional incinerators
are incomplete, they point to the possibility of some impact on the
environment in the immediate vicinity of the plant. Such assessment,
even if incomplete and based largely on modelling computations,
justify legislation restricting emission from MSW incinerators. Ad-
vanced control technology can markedly reduce the emission of metals
(Table 7 ) . The following considerations seem to be relevant in this
respect:

(a) the air concentrations (increase above background level)


in the immediate vicinity as compared with the urban back-

36
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

ground levels; here, the direct toxic action via inhal-


ation should be considered

(b) the indirect impact in the vicinity of the plant, the in-
dicators of which may be the increase of the concentration
in soil and plants grown for human consumption

(c) direct impact in the immediate vicinity on humans, as


judged by biological monitoring of human samples (e.g.
blood, urine, and hair)

(d) indirect impact at regional and global level, assessed by


comparing of emission sources of varying strength.

Populations under consideration

Two distinct populations can be identified when considering


exposure to refuse incinerator emissions. The first consists of
those individuals who are close to incinerator plants while the
second is the general population.

Populations close to incinerators

In many countries, refuse incinerators are located in densely


populated areas. Therefore, the identification of the potential
routes and intensity of exposure of local residents as a result of
emissions from these plants are pertinent. Unfortunately, little
information is available on the environmental levels of cadmium,
lead, mercury, and PAH around municipal incinerators. However, their
emissions could elevate air concentrations, deposition rates, and
soil and dust levels. The deposition of mercury is especially dif-
ficult to predict because of the mobility of this element in the
environment through re-vaporization that gives rise to the "bounce
off" effect reported for other point sources [102]. Mercury
emissions may increase mercury levels in local freshwater,
especially in water systems with low pH. Elevation of ambient air
levels of metals is unlikely to be large near advanced incinerator
plants for several reasons: stringent emission controls are imposed
on new incinerator plants; modelling data indicate minimal impact
around advanced incinerators; and high urban background values may
mask any contribution from refuse incinerators.
Air concentration increases will have to be relatively large to
increase noticeably total exposure levels, as the dietary intake of
these metals is normally greater than the respiratory intake. This
is particularly important for cadmium where even a doubling of urban
background levels (approximately 10 ng/m 3 ) would produce only
minor increases in total cadmium exposure.

37
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Deposition of cadmium, lead, and PAH onto soil and garden


vegetables around incinerators, either from stack emissions or fugi-
tive release, could increase dietary exposure. Once again, little
information is available.
Finally, street and possibly household dusts could contain ele-
vated concentrations of metals (cadmium and lead) and PAH as a
result of incinerator emissions. Lead levels in urban dust are
markedly elevated (approximately 1000 ug/g) compared with those of
rural dust, and incinerator emissions are unlikely to cause detect-
able increases, although fugitive releases may have an impact in the
immediate vicinity. The relative contribution of incinerators will
increase only when the use of unleaded petrol is widespread.

General population

The exposure pathway of relevance with respect to the general


population is dietary uptake. The tall stacks (commonly about 100 ra)
of modern incinerators will widely disperse and dilute the plume.
Thus, the metal and PAH emissions may contribute to the deposition
of these contaminants at considerable distances from the source. The
deposition of contaminants on agricultural land or in water systems
can have two effects: a long-term increase in the soil or sediment
concentration of the contaminant in question; and a direct depo-
sition onto crop plants and the subsequent ingestion of the contami-
nant. In the first case, if the soil level increases, the crop
level may also rise. This is the case for cadmium, but soil uptake
of lead and PAH by plants is considered to be less important than
direct deposition [103].
The question needs to be answered, however, whether inciner-
ation contributes significantly to the deposition of these contami-
nants at sites distant from point sources. Such an assessment re-
quires information on the emission strengths of other sources to
construct an inventory of atmospheric release. In the case of lead,
motor vehicle emissions dwarf incinerator emissions [104]'. There-
fore, this pathway is unlikely to be of current importance in Europe
for lead in crops. The situation for PAH is uncertain given the lack
of information. Only for cadmium is the pathway considered important
because of the relatively large discharges of this metal from in-
cineration [105].

Local health impact of cadmium

The Air Quality Guidelines for Europe [51] quote a concen-


tration of 2 ug/m3 of cadmium (2000 ng/m 3 ) as being likely to
cause, through life-long exposure, renal accumulation of this metal
sufficient to reach the critical concentration in the kidney. The
recommended levels were are <l-5 ng/m3 for rural areas and
10-20 ng/m for urban areas, with emphasis on the qualifying

38
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

statement that "an increase in present levels should not be tol-


erated".
Direct measurements of cadmium concentrations in the air close
to incinerators seem to be lacking. A rough estimate can be obtained
in two ways. One way is through modelling, in which one assumes for
the ground level a fraction of the cadmium concentrations directly
measured in the effluent gases. Such calculations, although burdened
with a high uncertainty, lead to the expected increase (over back-
ground levels) of the order of up to 80 ng/m3 for traditional in-
cinerators and less than 2 ng/m3 for advanced incinerators (Table
13). Such values, neither alone nor in combination with the back-
ground levels for urban areas, would be expected to lead to adverse
health effects by inhalation. The second way is through recomputing
the existing data on the rate of deposition. In a pathway analysis,
1 ng/m3 is estimated to cause a deposition of 1.6 g/ha/y [106].
Deposition rates of cadmium in the vicinity of an incinerator
[25] in a rural area of the Federal Republic of Germany were about
20 g/ha/y for a traditional incinerator, and half this value after
advanced control equipment was added. The first value corresponds
roughly to an ambient air concentration of 10 ng/m 3 . Further simi-
lar examples could be considered, but the conclusion would be valid
that these concentrations are at least one order of magnitude lower
than the critical dose for inhalation. The above example, if applied
to an urban area where the background concentrations of cadmium are
generally about 5 to 10 ng/m 3 , would lead to a concentration
between 10 and 20 ng/m 3 , and the conclusion remains valid.
The possible influence of incineration on environmental levels
of cadmium in the immediate vicinity of the plant has, until re-
cently, received little attention. Hutton et al. [107] record, in
the vicinity of a traditional incinerator in the London area, depo-
sition rates of about 3 to 70 g/ha/y in the downwind area as com-
pared with 1 to 16 g/ha/y in the upwind area. This deposition has
not, after 15 years of operation, markedly elevated cadmium in
either street dust, soil, or grass as compared with the upwind area
and other London locations. Studies summarized by Brunner & Zobrist
[30] reported elevated levels of cadmium in spinach grown near two
refuse incinerators, though only trace quantities were detected in
grass samples near other plants.
At present, the evidence does not indicate that the level of
contamination of the environment by cadmium in the immediate vici-
nity of incinerators has created a health hazard. However, only
limited data are available and this situation may change with time.
Therefore, locally grown food should be periodically monitored for
cadmium levels.

39
EHISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Local health impact of mercury

Urban ambient air concentrations of mercury are usually in the


range of 4 to 5 ng/m3 [55]. For occupational exposure, a concen-
tration in air of 50 ug/m3 is allowed. For non-occupational ex-
posure, the outdoor and indoor air concentrations of mercury are
proposed to be safe (with an appreciable safety factor) at 1 ug/m3
[51].
The concentrations of mercury in ambient air in the vicinity of
incineration plants have not been monitored. However, concentrations
are unlikely to exceed 100 ng/m3 (see Table 13) and cannot be con-
sidered of direct importance to the health of the inhabitants, ir-
respective of age, sex, and health status.
Inclusion of mercury in this report is based solely on one
pathway. This involves deposition of mercury from the atmosphere
onto soil and into surface waters: only the latter is relevant.
Here, through conversion into methylmercury, it accumulates in fish
that are eaten by people.
The only situation in which this pathway could have local im-
pact is an area with rivers or lakes in the vicinity where fishing
is an important activity and where the fish are consumed locally.
The exposure assessment will be constrained by several factors, such
as the history of past contamination of the area from other sources
(as mercury in the lake sediments has a long residence time) and the
background of the given area (region) dependent on the global mer-
cury cycle, which basically dominates the deposition of the metal.
Another confounding factor, however, is the acidification of surface
waters increasing in parallel with the overall contamination of am-
bient air from anthropogenic sources, enhancing the solubility of
mercury deposits [102].

Local health impact of lead

Inhalation represents an important source of lead uptake for


the general adult population. Uptake by inhalation is in the range
of 20 to 70% of the total, depending on the ambient air concen-
tration. Based on the assumed total uptake, the Air Quality Guide-
line value for lead in ambient air is 0.5 to 1.0 ug/m3 and this
includes a safety factor of about 2 [51].
The ambient air levels of lead in European areas vary from
0.1 to 0.3 ug/m3 in rural areas and from 0.5 to 3.0 ug/m3 in
most European cities [51]. The degree to which waste incineration
increases these concentrations is not known, and some estimates
could be made only from modelling data and the few existing data on
lead deposition rates.
In rural areas of the Federal Republic of Germany, the back-
ground deposition rate of lead is 150 g/ha/y, whereas downwind at <1
km of an incinerator, this value is 500 g/ha/y for the traditional
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

type and about 275 g/ha/y for the same plant after modernization
[25]. Assuming that these data on lead concentrations in ambient air
in rural areas are of the order of 0.1 ug/m 3 , the lead levels near
an incinerator (located in a rural area) could be of the order of
0.2 to 0.3 ug/m3. Such values, if applied to an urban area, would
elevate the background levels by some 0.1 to 0.2 ug/m 3 . Thus,
waste incineration alone does not seem likely to cause locally
significant elevations of the ambient air lead concentration
sufficient to lead to health effects by inhalation.
Other available data [107] do not point to significantly ele-
vated levels of lead in street dust, soil, or grass in the vicinity
of an incinerator in the London area. No impact on human health
from the deposition of lead from incinerators onto locally grown
food is expected.
For children, general contamination of the environment (e.g.
street dust and soil) may play a dominant role in their exposure
pattern. At present, the increased exposure derived from incinerator
emissions via this pathway cannot be quantified but it is not ex-
pected to play a major role in urban areas.
To summarize, in general no local health impact of lead from
incinerator emissions alone should be envisaged. The relative signi-
ficance of lead emissions from incinerators to total exposure levels
among local populations will be greater in more rural areas, where
other sources, particularly motor vehicle emissions, make a smaller
contribution.

Contribution of incinerator emissions to metal exposure in the


general population

This section assesses the extent to which MSW incineration in-


fluences metal exposure in the general population. The issues of
concern are the fate and significance of the long-range transport of
emitted metals and the metal build-up in soils and sediments in
rural areas.

Mercury

Fish consumption is by far the major source of methylmercury


exposure in the general population. In most countries, marine fish
are the dominant source but in some countries, freshwater fish are
also regularly consumed. MSW incineration is a significant source of
inorganic mercury in the atmosphere, but in most industrialized
countries, coal combustion and other sources (e.g. chlor-alkali
works) dominate. Nevertheless, MSW incineration is expected to make
an important contribution to the mercury cycle at the regional and
global level. What is not clear, however, is the significance of
this perturbation on the behaviour and accumulation of methylmercury
in edible fish species. Direct discharges of inorganic mercury to

41
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

aquatic systems are expected to be more important in this respect


and to conceal any effect from atmospheric inputs, at least in the
short term. Continued release of large quantities of airborne mer-
cury by human activities may progressively increase concentrations
of mercury in freshwater and possibly marine systems. If this is the
case, MSW incineration is only one contributor to the overall
anthropogenic total of airborne mercury; coal combustion is much
more important.

Cadmium and lead

The issue of concern is whether airborne emissions of cadmium


and lead from MSW incineration bring about significant atmospheric
inputs of these two metals to agricultural land. For both metals,
dietary intake is a major source of exposure for the general popu-
lation. Even in rural areas, direct atmospheric deposition is an
important source of lead in certain crop species [108].
However, most of the lead deposited in such areas is derived
from petrol combustion [104]. Thus, refuse incineration will make
only a minor contribution to lead levels in crops in rural areas.
For cadmium, the situation is different because, in contrast to
lead, plants take up cadmium relatively efficiently from the soil
[103]. Thus, the accumulation of cadmium in agricultural soils is of
particular concern as this can lead to enhanced crop concentrations
and hence increases in dietary intake for the general population.
Important sources of cadmium inputs to arable land are phosphate
fertilizers and atmospheric deposition. At local level, sewage
sludge application is also important. In the United Kingdom, one
third of the contribution from atmospheric deposition is estimated
to originate from MSW incineration [103].
Many countries have taken steps to reduce cadmium emissions,
while others are trying to prevent any increases in the average
dietary exposure to the metal. At the same time, countries are in-
creasingly recognizing that, in contrast to lead, the multiple
source nature of cadmium necessitates control measures on a wide
range of sources to reduce effectively inputs to agricultural land.
In view of this, refuse incineration is considered by several
authorities to be a sufficiently large source of cadmium to merit
further controls.

Environmertal release of metals from refuse incineration compared


with other sources

Numerous human activities result in the environmental release


of potentially toxic trace elements. The identity of these sources
is well known, and attempts have been made in recent years to assess
their quantitative importance. Such studies have been carried out at
the local level for a single city or county as well as at the
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

regional and global level. The inventories produced by these in-


vestigations provide an insight into the relative importance of
traditional refuse incineration as an environmental source of metal
release. These studies refer to emissions from traditional MSW in-
cinerators; the contribution from incineration to overall metal
emissions will decline as incinerators of advanced design become
widely used.

Environmental release of metals in the United Kingdom

About 34 x 10 s t of MSW are generated annually in the United


Kingdom, of which about 10% is incinerated. Emission factors (gram
metal released per tonne material consumed) were derived from ex-
perimental in-stack studies of incinerators in Europe and the USA.
Table 16 shows the resulting atmospheric emission discharges. The
residual trace metal burdens associated with the fly ash and furnace
clinker are landfilled. Table 16 also shows the estimated quantities
of the trace metals present in the remaining 90% of the MSW that is
landfilled directly.
The data in Table 16 may be compared with the inventories of
trace metal release to the atmosphere and landfill for all anthropo-
genic sources in the United Kingdom. In the case of cadmium,
Table 17 indicates that traditional refuse incineration is the
single largest source of atmospheric release, being responsible for
about one third of the total. Atmospheric lead discharges are also
considerable from traditional incineration, being greater than
emissions from nonferrous metal production. Nevertheless, lead
emissions from petrol combustion currently dwarf all other sources
of lead. Mercury emissions from incineration account for about one
tenth of the total anthropogenic discharge in the United Kingdom.

Table 16. Environmental release of trace elements from municipal


vaste disposal in the United Kingdom, 1983 [103]

Disposal route Trace elements release (t/y)


Cadmium Lead Mercury

Direct landfill 479 31 673 62.0

Incineration
Atmosphere 5 142 5.9
Landfill 46 3 241 0.7

43
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

The landfill inputs of metals in Table 16 reveal the much larger


tonnage associated with the direct disposal of MSW compared with the
incinerator residues. However, the latter is likely to be of greater
environmental significance at a local level because trace elements
are generally present at much higher concentrations.

Environmental release of metals in Sweden

Several emission inventories have been carried out in Sweden in


the last 5 years. A detailed investigation into the sources of at-
mospheric mercury is summarized in Table 18. These data indicate
much smaller total emissions of mercury in Sweden than in the United
Kingdom. In addition, refuse incineration emerges as a more im-
portant source of atmospheric mercury, mainly because of the rela-
tively small quantity of coal combusted in Sweden. Refuse inciner-
ation accounted for over half the total released in 1985 [45]. The
release of other metals from MSW incineration was less significant,
accounting for only 0.3X of the total cadmium emissions.
As a result of a national programme for collecting used bat-
teries and installing advanced flue gas treatment at some plants,
the emission of mercury from waste incineration in Sweden is ex-
pected to be reduced from 3.3 t/y (Table 18) to about 1 t/y from
1987 (K. Hasselgren, personal communication, 1987).

Table 17. Estimated atmospheric emissions of trace elements in the


United Kingdom [103]

Source Atmospheric emission (t/y)


Cadmium Lead Mercury

Nonferrous metal production 3.7 51 5.0


Production and use of
articles containing the
element ND1 6802 10.1
Iron and steel production 2.3 478 1.8
Fossil fuel combustion 1.9 80 25.5
Cement manufacture 1.0 36 2.5
Municipal waste incineration 5.0 142 5.9
Sewage sludge incineration 0.2 1.2 0.6

Total 14.1 7590.2 51.4

ND = not determined.
Atmospheric emission not determined but probably negligible.

44
EMISSIONS OF HEAVY METAL AMD PAH COMPOUNDS

Table 18. Estimated emissions of mercury to die in Sweden. 1984


[45]

Source of emission Emission of mercury


kg/y

Combustion of coal and peat 200


Chlor-alkali industry 400
Crematoriums 300
Smelting (mainly copper and zinc) 900
Incineration of household waste 3300
Other 200

Total 5300

Cadmium release in the European Community

A cadmium inventory survey was carried out in 1980 for the then
nine Member States of the EEC [105]. Table 19 presents a breakdown
of the amounts of MSW incinerated, and the estimated discharges of
cadmium to landfill and the atmosphere. Atmospheric emissions of
cadmium from traditional refuse incineration were estimated to ex-
ceed 30 t in 1977; the largest contributors were, in decreasing
order, the Federal Republic of Germany, France, and the United King-
dom. In comparison with other human activities and natural sources,
traditional refuse incineration emerges as a major source of atmos-
pheric release of cadmium, being responsible for about 25% of the
regional total, and is the second largest single source category.

Hetal release at the global level

Nriagu [109] estimates the total worldwide atmospheric emissions


of several metals from human activities. Host of this information is
not available at present, but Table 20 summarizes the reported
emission strengths for cadmium. Traditional refuse incineration
also makes a considerable input to the global release of cadmium,
being the largest single source after the nonferrous metal
industries.

Emissions of metals other than cadmium, mercury, and lead

In addition to the three metals covered in this report,


emissions from municipal incinerators, in common with many com-
bustion processes, will contain trace quantities of several other
metals. Traditional MSW incineration may be responsible for major

45
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 19. Quantity of incinerated refuse and estimated discharges


of cadmium in the European Community* in 1977 [105]

Country Waste Cadmium in discharge


incinerated medium (t)
(x 10' t) Atmospheric Ash
emissions

Belgium 0.5 0.8 7.3


Denmark 2.5 3.7 33.8
France 4.9 7.4 66.0
Germany, Federal -
Republic of 5.4 8.1 72.9
Italy 2.6 3.9 35.1
Luxembourg 0.1 0.2 1.4
Netherlands 1.7 2.6 23.0
United Kingdom 3.2 4.8 43.0

Total 20.9 31.5 282.5

• Except Ireland.

Table 20. Worldwide anthropogenic; emissions of cadmium to the at-


mosphere [109]

Source Annual release


(103 t/y)

Mining and production of nonferrous metals 4.71


Secondary nonferrous metal production 0.60
Iron and steel production 0.07
Industrial applications 0.05
Coal combustion 0.06
Waste incineration 1.40
Other sources 0.23

Total 7.12

46
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

fractions of zinc, antimony, silver, indium, and tin found in urban


aerosols [17].
Some compounds of inorganic arsenic, hexavalent chromium, and
nickel have caused lung cancer after occupational exposure to very
high concentrations [51]. Such compounds are suspected of being
potential carcinogens for the general population, even at the low
concentrations found in ambient air. However, based on the emission
data, the emissions of such compounds from incinerators would prob-
ably contribute very little to ambient air levels. If there is a
risk for lung cancer from ambient air levels, the additional risk
from incinerator emissions would not be of any practical signifi-
cance .

Contribution of incinerator emissions to PAH exposure

This section considers the relative importance of MSW inciner-


ation as a source of human exposure to PAH. As the data on PAH
other than BaP are severely limited, this discussion is restricted
mostly to BaP.

Direct exposure via inhalation

The background concentrations of BaP quoted in the Air Quality


Guidelines [51] range from less than 1 ng/m3 in rural areas, less
than 10 ng/m3 in urban areas, and up to 40 ng/m 3 in industrial
areas. The last value was recorded in the vicinity of a coke oven
plant.
The concentrations of BaP reported in stack gases of inciner-
ators range from less than 1 ng/m3 for advanced facilities and to
60 ug/m3 for traditional incinerators (Table 14). Maximum ground-
level concentrations of pollutants from individual incinerator plant
emissions can be estimated by using mathematical models. These
models attempt to allow for several aspects, such as the stack
height, local topography, and meteorological conditions in the given
area. However, these models have yet to be validated by comparing
the estimated concentrations with measurements taken in the field.
A simple dilution factor of 5 x 10" s [24] may be applied to
the stack gas emissions of incinerators to gauge the order of magni-
tude of ambient air concentrations of BaP at ground level. On this
albeit simplistic basis, the worst case emission of BaP given in
Table 14 (208 ug/m 3 ) for traditional incinerators would result in
a maximum ambient air concentration at ground level of 10 ng/m 3 .
This is somewhat less than the concentration of BaP recorded in the
vicinity of a coke oven plant [51]. However, for most incinerators
of traditional design cited in Table 14, the maximum ambient air
concentration of BaP at ground level is likely to be less than 10
ng/m3 (Table 13), which is similar to the background concen-
trations in urban ambient air.

47
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Most MSW incinerators are situated in urban areas, so the esti-


mated maximum concentrations of PAH at ground level should be added
to the prevailing background values. On the basis of the worst-case
examples presented here, a poorly operated incinerator of tradi-
tional design may, at most, double the ambient air concentration of
PAH. However, the impact of most traditional incinerator plants
will likely be much less.
The stack emission data for advanced incinerators (Table 14)
show PAH concentrations considerably less than the background con-
centrations in urban ambient air. This type of incinerator is
therefore most unlikely to increase PAH concentrations in air close
to the plant. Some recent field measurements also support this con-
clusion [110]. These workers recorded a maximum concentration of BaP
in air at ground level of less than 1 ng/m 3 , measured at two
sampling sites situated 900 m and 2500 m from an incinerator. Most
values recorded were less than 0.4 ng/m 3 , and days with peak
values of PAH in the ambient air were not correlated to days with
peak PAH values in the stack gases of the incinerator plant. What
type of incinerator was examined in this study is not clear, but if
it were of the traditional type, it would only strengthen the con-
clusion that advanced incinerators will have little, if any, impact
on ambient air levels of PAH.

Mutagenic activity in emissions

Besides analysis of specific chemical components in the flue


gas, the biological activity may also be tested, thereby offering
complementary information on potential health effects. The Sal-
monel2a/microsomal assay has been used to detect mutagenic activity
in the emissions from different combustion sources, including MSW
incineration and ambient air [111-113].
The mutagenic activity is distributed between fractions con-
taining PAH and more polar fractions, probably containing oxygenated
PAH components [113]. Thus, other substances besides unsubstituted
PAH are of importance. As the identity of these compounds is not
known, their potential health impact cannot be assessed.
Technical measures aimed at optimizing the combustion efficiency
may reduce the emission of mutagenic substances, as well as the
emission of other organic compounds. The results from mutagenicity
testing can be used, for example, to compare the effect of different
control devices on emissions, especially in combination with chemi-
cal analyses. However, the data generated with the Salmonella/-
microsomal assay are insufficient to estimate the mutagenic potency,
and even less the carcinogenic risks of various emissions. On its
own, this test can give only an insight into the potential for
mutagenicity; it cannot produce quantitative data.
EHISSIONS OF HEAVY HETAL AND PAH COHPOUNDS

Indirect exposure via deposition onto food crops

The estimated increase* in the deposition rate of PAH in the


vicinity of MSW incinerators (Table 13) is 0.02 to 1.5 g/ha/y. The
influence of this small increase in deposition of PAH may slightly
increase the PAH concentrations in food crops grown in the vicinity
of a traditional incinerator, particularly one poorly situated with
respect to the local geography. However, this source is not expected
to increase appreciably the total daily intake of PAH.

Emissions of PAH from MSW incinerators compared with other sources

Table 21 shows that incineration and open burning of refuse con-


tributes about 25X of the global BaP emissions to the atmosphere.
The emissions from open burning of refuse and agricultural wastes
will heavily outweigh the contribution from MSW incinerators, which
together make up this estimate.
More recent estimates for the Nordic countries (Table 22) in-
dicate that the contribution of MSW incinerators to emissions of PAH
is probably less than 5X of the total. In Norway, aluminium smelting
is the largest single source, whereas in Denmark, agricultural
burning is the dominant source. If agricultural burning, forest
fires, and industrial emissions are excluded, residential heating
with wood contributes from 44 to 68X of the total emission in dif-
ferent countries. Motor vehicles is the other dominant source.

Table 21. Estimated emissions of BaP to the atmosphere [114]

Source BaP in t/y


USA Worldwide Worldwide
(excl. USA)

Heating and power


generation 475 2 129 2 604
Industrial processes 198 847 1 045
Refuse and open burning
including incinerations 588 762 1 350
Vehicles 22 23 45

Total 1 283 3 761 5 044

Contribution from
incineration (X) 46 -20 27

49
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Table 22. Estimated emissions of PAH from different sources in the


Nordic countries (kg/y) [115]

Source Norway Sweden Denmark Finland

Residential combustion 49 000 105 000 29 000 42 000


(wood, oil, gas)

Industrial production 230 000* 48 000 1 200 2 700

Power and heat generation


(coal, oil, biomass) 230 6 600 550 1 100
Municipal incineration 250 2 200b 3 500 170

Open burning, forest fires


agricultural burning 13 000 7 800 33 000 5 500

Mobile sources
(gasoline and diesel
automobiles) 20 000 47 000 22 000 26 000

Total 312 480 216 600 89 250 77 470

Contribution from waste


incineration (X) 0.08 1.0 4.0 0.22

* 180 000 kg from aluminium production.


b
Later estimated to be 840 kg/y [45].

CONCLUSIONS AND RECOMMENDATIONS

Conclusions

1. Cadmium, lead, and mercury are the metals of prime concern


because of their toxicity and the relative importance of municipal
solid waste (MSW) incineration as a source of these metals emitted
to the atmosphere. Considerable amounts of these metals may be
emitted from incinerators of traditional design, which in turn may
increase exposure among residents in the vicinity of such an in-
cinerator.

50
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

2. As most MSW incinerators in operation are of traditional design,


they are an important source of cadmium and mercury emissions to the
atmosphere at a regional level and can contribute to the total human
intake of these metals through the food chain. However, the contri-
bution of lead from incinerators through this pathway is negligible
in comparison with emissions from other sources, such as motor vehi-
cles and smelters.

3. Incinerators can be designed and operated in a manner that will


affect the physical and chemical properties of metallic combustion
products and their distribution into bottom ash, boiler ash, fly
ash, and stack emissions. Emissions of metals, such as cadmium,
lead, and mercury, can be considerably reduced by use of a proper
flue gas cleaning system.

4. On the basis of the limited data available, metal emissions from


advanced MSW incinerators may not increase exposure levels in the
population living near such facilities.

5. Advanced air pollution control systems result in increased


quantities of dry or wet residues. Gas treatment residues, quench
waters, and other liquid effluents require appropriate treatment
prior to disposal.

6. Management of MSW incinerator residues must be done properly to


prevent dispersal of ashes by fugitive emissions and contamination
of surface and groundwaters due to the leachability of metals,
particularly cadmium and lead.

7. The level of PAH emissions from MSW incinerators varies widely,


and the factors causing these variations are not thoroughly under-
stood. Nevertheless, tests show that advanced incinerators operating
at sufficiently high temperatures and with adequate oxygen, good
mixing, and adequate retention time (together reflecting good com-
bustion conditions) result in lower formation levels of PAH than in
traditional incinerators and much lower than in poorly maintained
and poorly operated incinerators. The data on advanced incinerator
designs indicate that highly efficient destruction of PAH can be
achieved in a single-chamber incinerator.

8. The available data indicate that advanced MSW incinerators will


make only a minor contribution to the PAH concentrations in ambient
air.

9. At a local level, poorly operated MSW incinerators may, in the


worst case, increase the ambient air concentration of PAH in urban
locations by a factor of 2, and, consequently, may add to the risk
of cancer induction. Furthermore, the likelihood of PAH contami-

51
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

nation of food crops in the vicinity of such incinerators cannot be


excluded. However, PAH are only a fraction of the potentially toxic
organic compounds emitted from incinerators.

10. At a regional level, MSW incineration makes only a small (up to


a few percent) contribution to the total PAH emission and is there-
fore of minor importance compared with other sources.

Recommenda t ions

1. The local environmental impact of MSW incinerators should be


investigated at a few selected facilities by direct determination of
cadmium, mercury, lead and PAH concentrations in air, deposited
dust, soil, and vegetation. These values should be compared with
appropriate background values. Studies should also be conducted at
ash residue landfill sites, with particular reference to the poten-
tial contamination of surface and groundwaters by metal leachates.

2. Major sources of metals in MSW, such as cadmium, lead, and mer-


cury, should be identified, their amounts evaluated, the signifi-
cance of their removal on incineration emissions assessed, and al-
ternative disposal routes investigated.

3. The evaluation of metal and PAH emissions should be based on a


series of measurements of emissions from MSW incinerators, and the
recording of corresponding operating conditions of the incinerator
and flue gas cleaning devices and MSW characteristics.

4. Additional studies should be conducted to validate sampling


techniques and analytical methods for the measurement of PAH and
metal emissions, especially mercury, from incinerators.

5. A better and more comprehensive scientific database should be


developed to refine criteria for the selection of operating con-
ditions for traditionally designed incinerators to control more ade-
quately PAH emissions from such facilities.

6. Many PAH are known animal carcinogens and may also be carcino-
genic to humans. As the cancer risk from carcinogenic PAH is assumed
to depend on dose, the emissions of these substances, even at low
levels over a prolonged time, should be kept to a minimum.

7. Substituted PAH compounds emitted from MSW incinerators, such as


methylated, nitrated, and oxygenated PAH, and organic compounds
other than PAH, should be identified and their biological effects
investigated.

52
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

8. Investigations should be continued to increase combustion


efficiency that would, in turn, maximize the destruction of organic
compounds and their conversion to carbon dioxide.

9. Advanced technologies of MSW incinerators and emission control


systems should be implemented rapidly to reduce environmental dis-
persal of metals and PAH.

10. Application of genotoxicology testing in conjunction with chemi-


cal analysis should be considered as a valuable tool for assessing
the impact of operating conditions and new technologies on the
potential toxicity of pollutant mixtures emitted in the stack gas.

11. The location of new MSW incinerators should be carefully


selected to minimize human and environmental impact from metal and
PAH emissions.

12. Safe handling of ash residues, both in the incinerator plant and
during transport to disposal sites, should be practised to minimize
occupational exposure and fugitive emissions; assessments of the
metal and PAH exposure levels of the operators should be undertaken.
Liquid effluents from wet scrubbers and quenches should be properly
treated prior to discharge to receiving waters.

13. The construction of small incinerators should be discouraged


when adequate number of properly trained personnel cannot be pro-
vided on a cost-effective basis, and should be permitted only when
proper pollution control equipment is incorporated in the inciner-
ator facility.

REFERENCES

1. PCDD and PCDF emissions from incinerators for municipal sewage


sludge and solid waste - evaluation of human exposure. Copen-
hagen, WHO Regional Office for Europe, 1987 (Environmental
Health Series, No. 17).

2. Patrick, P.K. Glossary on solid waste. Copenhagen, WHO Regional


Office for Europe, 1980.

3. Buekens, A. & Patrick, P.K. Incineration. In : Suess, M.J., ed.


Solid waste management: selected topics. Copenhagen, WHO
Regional Office for Europe, 1985.

A. Seeker, W.R. et al. Municipal waste combustion study; com-


bustion control of organic emissions. Research Triangle Park,
NC, US Environmental Protection Agency, 1987.

53
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

5. Churney, K.L. et al. The chlorine content of municipal solid


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EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Annex 1

MEMBERSHIP OF SUBGROUPS

Subgroup 1: Incineration of municipal solid waste

Dr Brunner Dr Romanelli
Mr Finkelstein (.Leader) Mr Smith
Mr Kilgroe Mr Velzy (Rapporteur)
Mr Milhau Dr Viviano
Mr Moller Dr Vogg
Dr Nottrodt Mr Woodfield

Subgroup 2: Environmental pathways and impact on health

Dr Bencko Dr Riolfatti
Dr Borneff Dr Schoeny
Dr Dolara Ms Victorin
Dr Heinrich Dr Wadge (Rapporteur)
Dr Hutton Dr van Wijnen
Dr Kostial (Leader) Dr Zapponi
Dr Piotrowski

Subgroup 3: Conclusions and recommendations

Mr Finkelstein Dr Suess
Dr Kostial Mr Velzy (Co-Rapporteur)
Dr Piscator (Leader) Dr Wadge (Co-Rapporteur)
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Annex 2

LIST OF PARTICIPANTS

Temporary advisers

Dr Vladimir Bencko, Senior Research Worker, Postgraduate School of


Medicine and Pharmacy, Prague, Czechoslovakia

Dr Joachim Borneff, Professor and Director, Institute of Hygiene,


University of Mainz, Federal Republic of Germany

Dr Paul H. Brunner, Senior Research Associate, Swiss Federal Insti-


tute for Water Resources and Water Pollution Control (EAWAG), Duben-
dorf, Switzerland

Dr Piero Dolara, Professor, Department of Pharmacology, University


of Florence, Italy

Mr Abe Finkelstein, Head, Refuse and Heating Section, Urban Activi-


ties Division, Environment Canada, Ottawa, ON, Canada (Vice-C/iair-
man)

Dr Uwe Heinrich, Head, Department of Experimental Environmental


Hygiene, Fraunhofer Institute of Toxicology and Aerosol Research,
Hanover, Federal Republic of Germany

Dr Malcolm Hutton, Deputy Director, Monitoring and Assessment


Research Centre (MARC), King's College, University of London, United
Kingdom

Mr James D. Kilgroe, Manager, Municipal Waste Combustion Program,


Air and Energy Engineering Research Laboratory, US Environmental
Protection Agency (US EPA), Research Triangle Park, NC, USA

Dr Krista Kostial, Professor and Head, Department of Mineral Meta-


bolism, Institute for Medical Research and Occupational Health,
Zagreb, Yugoslavia (Vice-chairman)

Mr Alain Milhau, Head, Air Pollution Control Department, French Air


Quality Agency, Paris, France

Mr Jens T. Mbller, Research Manager, Industrial Flue Gas Cleaning,


Air Pollution Control Division, Niro Atomizer A/S, Soborg, Denmark

Dr Adolf Nottrodt, President, Goepfert, Reimer and Partner Engineer-


ing Consultants, Ltd., Hamburg, Federal Republic of Germany

65
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Dr Jerzy K. Piotrowski, Professor and Head, Department of Toxico-


logical Chemistry, Institute of Environmental Research and Bioanaly-
sis, Medical Academy, Lodz, Poland

Dr Magnus Piscator, Professor, Department of Environmental Hygiene,


The Karolinska Institute, Stockholm, Sweden (Chairman)

Dr Massimo Riolfatti, Associate Professor, Institute of Hygiene,


University of Padua, Italy

Dr Mario Romanelli, Chemist, Air Pollution Sector, Environmental


Section, Department of Social Security, Regional Government of Tus-
cany, Florence, Italy

Dr Rita Schoeny, Toxicologist, Environmental Criteria and Assessment


Office, Office of Research and Development, US Environmental Pro-
tection Agency (US EPA), Cincinnati, OH, USA

Mr Anthony J. Smith, Principal Inspector, Department of the Environ-


ment, London, United Kingdom

Mr Charles 0. Velzy, President, Charles R. Velzy Associates, Inc.


(wholly owned subsidiary of Roy F. Weston, Inc.), Consulting En-
gineers, Armonk, NY, USA (Co-Rapporteur)

Ms Katarina Victorin, Toxicologist, Unit of Toxicology, National


Institute of Environmental Medicine, Stockholm, Sweden

Dr Giuseppe Viviano, Researcher, Air Unit, Environmental Health


Laboratory, National Institute of Health (ISS), Rome, Italy

Dr Hubert Vogg, Professor and Director, Laboratory for Isotope Tech-


nology, Nuclear Research Centre, Karlsruhe, Federal Republic of Ger-
many

Dr Andrew Wadge, Senior Scientific Officer, Division of Toxicology


and Environmental Health, Department of Health, London, United King-
dom (Co-Rapporteur)

Dr Joop H. van Wijnen, Regional Environmental Health Officer, Public


Health Department, Municipal Health Service, Amsterdam, Netherlands

Mr Michael J. Woodfield, Senior Scientific Officer, Pollution Abate-


ment Division, Warren Spring Laboratory, Stevenage, United Kingdom

66
EMISSIONS OF HEAVY METAL AND PAH COMPOUNDS

Dr Giovanni A. Zapponi, Senior Scientist and Director, Risk Assess-


ment Unit, Comparative Toxicology and Ecotoxicology Laboratory,
National Institute of Health (ISS), Rome, Italy

WHO Regional Office for Europe


Dr Michael J. Suess, Regional Officer for Environmental Health
Hazards (Scientific Secretary)

67

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