European Commission

14
KH-40-01-448-EN-N
Pollutants in urban waste
water and sewage sludge

ISBN 92-894-1735-8
OFFICE FOR OFFICIAL PUBLICATIONS
OF THE EUROPEAN COMMUNITIES

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Luxembourg: Office for Official Publications of the European Communities, 2001

ISBN 92-894-1735-8

© European Communities, 2001

Reproduction is authorised provided the source is acknowledged.
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 Executive Summary

Authors

I C Consultants Ltd London

Professor Iain Thornton

(scientific co-ordinator)

Dr David Butler

Paul Docx

Martin Hession

Christos Makropoulos

Madeleine McMullen

Dr Mark Nieuwenhuijsen

Adrienne Pitman

Dr Radu Rautiu

Richard Sawyer

Dr Steve Smith

Dr David White

Technical University Munich

Professor Peter Wilderer

Stefania Paris

IRSA Rome

Dr Dario Marani

Dr Camilla Braguglia

ECA Barcelona

Dr Juan Palerm

Pollutants in Urban Waste Water and Sewage Sludge 2

 Executive Summary

Table of Contents

EXECUTIVE SUMMARY 5

1. INTRODUCTION 9

1.1 INTRODUCTION TO POLLUTANTS IN URBAN WASTEWATER (UWW) AND

SEWAGE SLUDGE (SS)
1.2 OBJECTIVES AND GOALS

2. POTENTIALLY TOXIC ELEMENTS, SOURCES, PATHWAYS, AND FATE THROUGH

URBAN WASTEWATER TREATMENT SYSTEMS 13

2.1.SOURCES AND PATHWAYS OF POTENTIALLY TOXIC ELEMENTS IN UWW AND SS

2.1.1 DOMESTIC SOURCES
2.1.2 COMMERCIAL SOURCES
2.1.3 URBAN RUNOFF
2.2 INFLUENCE OF VARIOUS TREATMENT PROCESSES ON THE FATE OF
POTENTIALLY TOXIC ELEMENTS THROUGH WASTEWATER TREATMENT SYSTEMS
(WWTS) AND SEWAGE SLUDGE TREATMENT (SST)
2.3 QUANTITATIVE ASSESSMENT OF POTENTIALLY TOXIC ELEMENTS IN
UNTREATED UWW, TREATED UWW AND TREATED SS

3. ORGANIC POLLUTANTS: SOURCES, PATHWAYS, AND FATE THROUGH URBAN

WASTEWATER TREATMENT SYSTEMS 64

3.1. SOURCES AND PATHWAYS OF ORGANIC POLLUTANTS IN UWW AND SS

3.1.1 DOMESTIC AND COMMERCIAL
3.1.2 URBAN RUNOFF
3.2 INFLUENCE OF VARIOUS TREATMENT PROCESSES ON THE FATE OF ORGANIC
POLLUTANTS THROUGH WWTS AND SS
3.3 QUANTITATIVE ASSESSMENT OF ORGANIC POLLUTANTS IN UNTREATED UWW,
TREATED UWW AND TREATED SS

4. HEALTH AND ENVIRONMENTAL EFFECTS OF POLLUTANTS IN UWW AND SS 94

4.1 POTENTIALLY TOXIC ELEMENTS
4.2 ORGANIC POLLUTANTS

Pollutants in Urban Waste Water and Sewage Sludge 3

 Executive Summary

5. A REVIEW OF EU AND NATIONAL MEASURES TO REDUCE THE POTENTIALLY

TOXIC ELEMENTS AND ORGANIC COMPOUNDS CONTAMINATION OF UWW AND SS
102

6. CASE STUDIES 113

(A) PLATINUM GROUP METALS IN URBAN ENVIRONMENT
(B) SUSTAINABLE URBAN DRAINAGE
(C) POLLUTANT SOURCES AND LOAD FROM ARTISANAL ACTIVITIES IN URBAN
WASTEWATER (THE MUNICIPALITY OF VICENZA, INCL. GOLD JEWELLERY SHOPS)
(D) PHARMACEUTICALS IN THE URBAN ENVIRONMENT
(E) PERFUME COMPOUNDS IN WASTEWATER AND SEWAGE SLUDGE
(F) SURFACTANTS IN URBAN WASTEWATERS AND SEWAGE SLUDGE
(G) USE OF POLYELECTROLYTES; THE ACRYLAMIDE MONOMER IN WATER
TREATMENT
(H) CASE STUDY: LANDFILL LEACHATE
(I) PTE (POTENTIALLY TOXIC ELEMENTS) TRANSFERS TO SEWAGE SLUDGE
(J) EFFECT OF CHEMICAL PHOSPHATE REMOVAL ON POTENTIALLY TOXIC
ELEMENT CONTENT IN SLUDGE

7. REPORT SYNOPSIS, DISCUSSIONS AND CONCLUSIONS 205

7.1 COMMENTS, CHALLENGES AND STRATEGIES FOR THE NEXT FIVE TO TEN
YEARS
7.2 IDENTIFICATION OF GAPS IN THE AVAILABLE INFORMATION,
7.3 RECOMMENDATIONS FOR FURTHER RESEARCH
7.4 SUGGESTIONS

APPENDICES 232
APPENDIX A - URBAN WASTEWATER TREATMENT SYSTEMS (WWTS) AND SEWAGE SLUDGE
TREATMENT (SST) - EU AND REGIONAL ASPECTS
APPENDIX B - PHYSICO-CHEMICAL PROPERTIES OF SELECTED POLLUTANTS

DATABASES, REFERENCES

GLOSSARY AND ABBREVIATIONS

Pollutants in Urban Waste Water and Sewage Sludge 4

 Executive Summary

POLLUTANTS IN URBAN WASTE WATER AND SEWAGE SLUDGE

EXECUTIVE SUMMARY

Water policy in the European Union is aiming to promote sustainable water use and a major
objective of the new Water Framework Directive (2000/60/EC) is the long-term progressive
reduction of contaminant discharges to the aquatic environment in urban wastewater
(UWW). Sewage sludge is also a product of wastewater treatment and the Urban Waste
Water Treatment Directive (91/271/EEC) aims to encourage the use of sludge whenever
appropriate. Potentially toxic elements and hydrophobic organic contaminants largely
transfer to the sewage sludge during waste water treatment with potential implications for the
use of sludge although some may be emitted with the effluent water.

Inputs of metals and organic contaminants to the urban wastewater system (WWTS) occur
from three generic sources: domestic, commercial and urban runoff. A review of available
literature has quantified the extent and importance of these various sources and the inputs
from different sectors. In general, urban runoff is not a major contributor of potentially toxic
elements to UWW. Inputs from paved surfaces due to vehicle road abrasion and tyre and
brake-lining wear have been identified and losses from Pb painted surfaces and Pb and Zn
from roofing materials represent localised sources of these elements.

Platinum and Pd are components of vehicle catalytic converters and emissions occur as the
autocatalyst deteriorates. Catalytic converters are the main source of these metals emitted
to the environment and releases have increased with the expansion in use of autocatalysts.
Platinum group metals (PGMs) potentially enter UWW in runoff and transfer to sewage
sludge in a similar way to other potentially toxic elements. The Pt content in sludge is
typically in the range 0.1 – 0.3 mg kg-1 (ds) and the background value for soil is 1 µg kg-1.
PGMs are inactive and immobile in soil.

In contrast to potentially toxic elements, inputs of the main persistent organic pollutants of
concern, including: PAHs, PCBs and PCDD/Fs, to UWW are principally from atmospheric
deposition onto paved surfaces and runoff. Combustion from traffic and commercial sources
accounts for the major PAH release to the environment, although inputs from food
preparation sources also represent an important and often under-estimated contribution of
certain PAH congeners. PCDD/Fs are released during waste incineration and also by coal
combustion. Soil acts as a long-term repository for these contaminant types and
remobilisation by volatilisation from soil is an important mechanism responsible for recycling
and redistributing them in the environment. For example, the industrial use of PCBs was
phased out in Europe during the 1980s-1990s, but 90 % of the contemporary emissions of
PCBs are volatilised from soil. Since emission controls are already in place for the main
point sources and PAHs, PCDD/Fs or PCBs enter UWW principally from diffuse atmospheric
deposition and environmental cycling, there is probably little scope, from source control, to
further reduce inputs and concentrations of these persistent organic substances in UWW or
sewage sludge.

Being strongly hydrophobic these organic pollutants are efficiently removed during urban
wastewater treatment (WWTS) and bind to the sludge solids. However, the increasing body
of scientific evidence has not identified a potential harmful impact of these substances on the
environment in the context of the urban wastewater system. Therefore, on balance, the
importance of these contaminants in UWW and sewage sludge has significantly diminished
and there may be little practical or environmental benefit gained from adopting limits or
controls for PAHs, PCBs or PCDD/Fs in UWW or sewage sludge. This is emphasised further
by the high cost and specialist analytical requirements of quantifying these compounds in
sludge and effluent.

5
 Executive Summary

Potentially toxic element contamination of urban wastewater and sewage sludge is usually
attributed to discharges from major commercial premises. However, significant progress has
occurred in eliminating these sources and this is reflected in the significant reductions in
potentially toxic element concentration in sewage sludge and surface waters reported in all
European countries where temporal data on sludge and water quality have been collected.
However, potentially toxic element concentrations remain higher in sludge from large urban
wastewater treatment plant (WWTP) compared with small WWTP and they are also greater
in sludges from industrial catchments compared with rural locations. These patterns in
sludge metal content suggest that commercial sources may still contribute significantly to the
total metal load entering UWW. Indeed, recent regional surveys of metal emissions from
commercial premises confirm that further reductions in most elements could be achieved
from this sector. The primary targets for source control include health establishments, small
manufacturing industries (particularly metal and vehicle related activities) and hotel/catering
enterprises, as 30 % of medical centres and 20 % of the other types of activity could be
discharging significant amounts of potentially toxic elements in UWW. Mercury is a specific
case where compulsory use of dental amalgam separators, and substituting Hg with
alternative thermoreactive materials in thermometers, may be effective in reducing
discharges of this element to the WWTS wastewater treatment system .

Faeces contribute 60 – 70 % of the load of Cd, Zn, Cu and Ni in domestic wastewater and
>20 % of the input of these elements in mixed wastewater from domestic and industrial
premises. Faecal matter typically contains 250 mg Zn kg-1, 70 mg Cu kg-1, 5 mg Ni kg-1, 2 mg
Cd kg-1 and 10 mg Pb kg-1 (ds). The other principal sources of metals in domestic
wastewater are body care products, pharmaceuticals, cleaning products and liquid wastes.
Plumbing is the main source of Cu in hard water areas, contributing >50 % of the Cu load
and Pb inputs equivalent to 25 % of the total load of this element have been reported in
districts with extensive networks of Pb pipework for water conveyance. Adjusting water
hardness in order to reduce metal solubilisation from plumbing is technically feasible, but is
likely to be impractical at the regional scale necessary to significantly reduce metal
concentrations in UWW and sludge and may be unpopular with consumers in hard water
areas. The gradual replacement of Pb water pipes can be achieved during building renewal
and renovation programmes.

Reductions in domestic discharges of metals may be possible through increased public

awareness of appropriate liquid waste disposal practices and the provision of accessible
liquid waste disposal facilities. It may be impractical to eliminate the use of metals in body
care products when they are an important active ingredient, but advice and labelling could
be improved to minimise excessive use. Cadmium may be a contaminant present in
phosphatic minerals and removing phosphate from detergent formulations can reduce
associated potential discharges of Cd from domestic sources.

Detergent residues (e.g.nonyl phenol, NP), surfactants (e.g. linear alkyl benzene
sulphonates, LAS), plasticising agents (e.g. di-(2-ethylhexyl)phthalate, DEHP) and
polyacrylamide compounds, added to sludge to aid dewatering, are quantitatively amongst
the most abundant organic contaminants present in UWW and/or sewage sludge.
Dewatering agents based on polyacrylamide may contain traces of the potentially toxic
acrylamide monomer, but this is rapidly degraded and polyacrylamide itself is biologically
inactive. Detergent residues and DEHP are primarily of domestic origin and they are
effectively degraded during aerobic wastewater treatment and are not considered to
represent a potential environmental problem from the discharge of treated effluents to
surface waters. Anaerobic digestion is the principal method employed for stabilising sewage
sludge, but NP accumulates during anaerobic digestion, DEHP is not removed by this
conventional process and, although a significant amount of LAS is biodegraded, residues of
this substance remain because of the large concentrations initially present in raw sludge.
The inability to degrade detergent residues anaerobically and the large concentrations
present in sludge and UWW have prompted ecolabelling initiatives in a number of European
countries to influence consumer choice away from detergents containing these surfactants to

Pollutants in Urban Waste Water and Sewage Sludge 6

 Executive Summary

alternative products. This has been successful when supported by extensive public
awareness campaigning. For example, the market share for ecolabelled detergents in
Sweden increased to 95 % and the consumption of LAS has decreased to a similar extent.
Surfactant residues and plasticisers degrade quickly when added to aerobic soils. The
oestrogenic activity of NP is however, a principal concern and measures are proposed to
eliminate the discharge of this substance to UWW.

Natural and synthetic oestrogens are degraded in WWT, but trace amounts remain and
represent the main source of oestrogenic activity in treated effluents. Further work is
necessary to link these substances to oestrogenic responses in aquatic life, but it may be
necessary in future to consider the requirement for tertiary treatment processes (e.g.
ozonation) to eliminate these substances from treated effluents.

A number of other groups of organic compound are identified as being potentially resistant to
wastewater and sewage sludge treatment and the most significant of these are brominated
diphenyl ethers (PBDEs) and chlorinated paraffins. Further research is warranted, in
particular to assess the persistence and potential environmental significance of these
compounds. Synthetic nitro musks are used in perfumed products and traces may be
present in UWW and sludge. Little is known about the environmental fate of these
compounds, but effects on human health from this route seem unlikely given that the main
exposure route is through direct contact.

The degree of removal and biodegradation of pharmaceutical compounds during WWT

varies considerably, although many common analgesic drugs rapidly biodegrade. They are
soluble and transfer to sludge is only of minor concern. Significant amounts of prescribed
drugs are excreted from the body and controlling these inputs from the general population
would be impractical. However, the disposal of unused drugs into UWW should be reviewed
and alternative methods of disposal should be encouraged. The potential significance of
pharmaceuticals in the environment should be assessed in context of the major inputs and
presence arising from widespread veterinary administration of drugs to livestock and farm
waste disposal to land.

A general recommendation to protect the water and soil environment is that a hazard,
biodegradability and fate assessment should be required for all new synthetic chemicals,
irrespective of their purpose or end-use, to determine the potential from them to transfer to
UWW or sewage sludge and the subsequent implications for the environment. Specified
criteria regarding toxicity and biodegradation could be set for compounds that exhibit a
propensity to enter the WWTS and restrictions could be enforced regarding production and
use if these were not met. These decisions would need to balanced against the potential
benefits to health derived from the administration of pharmaceutical drugs.

Strategies aimed at controlling pollutant discharges can only focus on those sources that can
be identified and quantified. Published mass balance calculations indicate there is a high
degree of uncertainty regarding inputs of potentially toxic elements entering the WWTS.
Indeed, unidentified sources may contribute as much as 30 - 60 % of the total metal load
entering the WWTS, although more than 80 % of the Cd discharged is from identified inputs.
This apparent discrepancy could be related to difficulties in measuring the highly variable
inputs of metals in urban runoff and the underestimation of discharges from commercial
premises that have not been subjected to trade effluent control.

The European Commission has proposed a list of 32 priority and 11 hazardous substances
(COM/2001/17) with the aim of progressively reducing emissions and discharges of these
chemicals to the environment. Current developments also suggest that Zn, Cu and LAS may
be the most limiting constituents in sludge if the proposed maximum permissible
concentrations for these substances in soil (Zn and Cu) and sludge (LAS) are carried
through in the revised of Directive 86/278/EEC, but they are not listed as priority substances.
Consideration should be given to designating Zn, Cu and LAS as priority substances to

Pollutants in Urban Waste Water and Sewage Sludge 7

 Executive Summary

minimise their to UWW as far as is practicable and to ensure there is a consistent link and
approach to defining the environmental quality standards for sludge with those for
sustainable water use and contaminant discharge reduction.

The main identified priorities for future research relating to contaminant sources, fate and
behaviour in the WWTS are:

• To reduce the uncertainty in quantifying contaminant discharges to UWW by identifying

and surveying specific sources to determine the potential for controlling inputs
particularly from small commercial sources and medical establishments;

• To establish the extent and variability of contaminant entry into UWW by catchment
investigations in relation to precipitation frequency and changes in sludge quality;

• To critically and independently review the fate, behaviour, degradability, toxicity and
environmental consequences of alternative surfactant and plasticing compounds, in
collaboration with the related chemical manufacturing industries, to inform decisions of
the benefits and disadvantages of product substitution in detergent formulations and
plastics manufacture;

• To determine the extent of volatilisation-deposition cycling of persistent organic

pollutants in the environment, identifying the processes controlling the extent and
magnitude of diffuse inputs of these substances to UWW and to provide long-term
predictions of changes in release patterns and the consequences for UWW and sludge;

• To develop a consistent statistical and reporting protocol for national chemical

composition data presented in surveys of sewage sludge quality.

Pollutants in Urban Waste Water and Sewage Sludge 8

 1. Introduction

1. INTRODUCTION

The primary objective of this study is to determine the sources of pollution in urban
wastewater (UWW) treated in wastewater treatment systems (WWTS). This includes the
pollutants introduced into the UWW collecting system with run-off rainwater, from domestic
and small commercial sources. The pollutant contents in urban wastewater and sewage
sludge has been evaluated by review of the existing literature, in order that measures may
be proposed to reduce pollution at source.

1.1 Introduction to pollutants in urban wastewater

The pollutants of interest can be divided into two main groups;

• potentially toxic elements (PTEs) including cadmium (Cd), chromium (Cr III and Cr
VI), copper (Cu), mercury (Hg), nickel (Ni), lead (Pb) and zinc (Zn),

• organic pollutants including PAHs, PCBs, DEHP, LAS, NPE, dioxins (PCDD) and
furans (PCDF). Over 6,000 organic compounds have been detected in raw water
sources most of which are due to human activities. While some of these are highly
persistent, others are easily biodegradable in WWTS.

Other pollutants of interest are the metalloids, arsenic and selenium and the metal silver.
Platinum group metals (PGMs), and pharmaceuticals are covered in detail in case studies.

The sources of metal pollution in the wastewater system can be classified into three main
categories:
• Domestic,
• Light industrial (connected to the WWTS) and commercial,
• Urban runoff (which also encompass lithospheric and atmospheric sources).

Pollutants in Urban Waste Water and Sewage Sludge 9

 1. Introduction

Atmosphere wet & dry

deposition
deposition

Lithosphere

INDUSTRY

products

DOMESTIC Wastes Product wastes RUNOFF

UWW COLLECTING COMBINED UWW STORM UWW

Wastes
SYSTEMS COLLECTING SYSTEMS COLLECTING SYSTEMS

WASTEWATER
TREATMENT WORKS

Receiving
Water

Figure 1.1: Sources of pollutants in wastewater [after Lester, 1987]

A summary of the various inputs, outputs and pathways followed by water and associated
contaminants from both natural and anthropogenic sources encountered in urban
environments is shown in Figure 1.1. It depicts the drainage area as an open system [Ellis,
1986]. A more detailed urban catchment figure is included in Appendix A.

Wastewater contains many constituents and impurities arising from diffuse and point
sources. Large point sources are easily quantifiable and result from specific activities in the
area that are connected to UWW collecting systems. The contribution from small point
sources, such as households and small businesses, is much more difficult to identify and
quantify, compared to point sources which are usually regulated. UWW is also vulnerable to
illegal discharges of pollutants.

Diffuse sources, such as atmospheric deposition and road runoff have also been
characterised and this study will attempt to present an overview of the available information
in this area. Different methods have been used to estimate point sources and diffuse (non-
point) sources contributions to the pollution load [Vink, 1999]. Inventories of point and diffuse
sources, can link observed water quality trends to changes in socio-economic activities.

Pollutants in Urban Waste Water and Sewage Sludge 10

 1. Introduction

The type of pollutants and the magnitude of the outfall loadings are a complex function of:

• size and type of conurbation (commercial, residential, mixed)

• plumbing and heating infrastructure
• atmospheric quality, for example long range transport of pollutants
• factors affecting deposition of pollutants such as precipitation
• activity and intensity surface composition and condition
• urban land use
• traffic type and density
• urban street cleaning
• maintenance practices and stormwater controls
• specific characteristics of storm events
• accidental releases

A review of the sources and pathways of potentially toxic element pollutants in urban
wastewater is presented in Section 2.1 and for organic pollutants in Section 3.1

1.2 Objectives and Goals

The main goals of the study were:

• To determine the sources of potentially toxic elements and organic pollutants in

domestic, commercial, and urban run-off wastewater, which end up in the UWW
collecting system.
• To make a qualitative and quantitative assessment of the pollutants in urban
wastewater and runoff rainwater on the basis of the available data in the literature.
• To evaluate the percentage of inorganic and organic pollutants concentrated in
sewage sludge and the percentage of pollutants released in the environment with the
treated effluents.
• To review wastewater and sewage sludge treatment processes and possible
measures to prevent pollution at source. The most important practices to treat
wastewater and sewage sludge in Europe will be closely examined.
• Based on an overall assessment of the existing data from various sources, to identify
further research directions in those areas with insufficient data.

This report presents a thorough literature review and is primarily based on the analysis and
presentation of case studies from a wide variety of sources and test catchments across
Europe, covering a time range from 1975 to date. Databases used during this project are
listed in the reference section. As theoretical approaches, such as modelling of pollutant
sources and predicted concentrations, are scarce the report attempts to summarise the
monitoring, sampling and measurement of numerous studies, thus providing a concise
overview of pollution source types and concentration ranges. The reader must keep in mind
that there are significant differences between the experiments (in duration, location,
measurement methods, measurement targets and initial conditions), and thus conclusions
on mean or extreme values of pollutants will have to be drawn carefully.

Pollutants in Urban Waste Water and Sewage Sludge 11