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Atmospheric Environment 84 (2014) 189e197

Contents lists available at ScienceDirect

Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Estimation and characterization of gaseous pollutant emissions from


agricultural crop residue combustion in industrial and household
sectors of Pakistan
Muhammad Irfan a, Muhammad Riaz a, Muhammad Saleem Arif a, *,
Sher Muhammad Shahzad b, Farhan Saleem a, Naveed-ur -Rahman c, Leon van den Berg d, e,
Farhat Abbas a
a
Department of Environmental Sciences, Government College University Faisalabad, Faisalabad 38000, Pakistan
b
Department of Soil & Environmental Sciences, University College of Agriculture, University of Sargodha, Pakistan
c
Department of Environment, Health and Safety, Interloop Ltd., Faisalabad, Pakistan
d
Department of Aquatic Ecology & Environmental Biology, Faculty of Science, Radboud University Nijmegen, The Netherlands
e
B-WARE Research Centre, Nijmegen, The Netherlands

h i g h l i g h t s

 Energy crisis has resulted in increased combustion of crop residues in Pakistan.


 Emission attributes of rice husk, rice straw, corncobs and bagasse were estimated.
 Rice straw had significantly higher gaseous pollutant emission factors.
 Bagasse had the highest value of total emission of gaseous pollutants.
 Rice straw and bagasse had >90% share in total gaseous pollutant emissions.

a r t i c l e i n f o a b s t r a c t

Article history: A long-term energy crisis has resulted in increased combustion of biomass fuel in industrial and
Received 10 July 2013 household sectors in Pakistan. We report results of a study on the emission characteristics of rice husk,
Received in revised form rice straw, corncobs and bagasse since they are frequently used as biomass fuel and differed remarkably
14 November 2013
in physico-chemical and combustion characteristics. Emission concentrations and emission factors were
Accepted 18 November 2013
determined experimentally by burning the biomass fuel using a burning tower. Modified combustion
efficiency (MCE) of rice husk, rice straw, corncobs and bagasse was >0.97 indicating that combustion was
Keywords:
dominated by flaming mode. Emission factors of gaseous pollutants CO, CO2, NO2, NO, NOx and SO2 for
Biomass fuel
Gaseous pollutants
rice straw were calculated to be 17.19  0.28, 1090.07  24.0, 0.89  0.03, 1.48  0.04, 3.16  0.08 and
Emission factors 0.38  0.03 g kg1 respectively which were significantly (p < 0.05) higher compared to those from rice
Emission allocations husk (14.05  0.18, 880.48  8.99, 0.19  0.01, 1.38  0.02, 2.31  0.04 and 0.11  0.03 g kg1), corncobs
Emission inventory (8.63  0.12, 595.44  10.38, 0.16  0.01, 0.70  0.01, 1.23  0.02 and 0.02  0.00 g kg1) and bagasse
(12.39  0.08, 937.03  9.07, 0.36  0.03, 1.44  0.02, 2.57  0.04 and 0.18  0.02 g kg1). Total emissions
of CO, CO2, NO2, NO, NOx and SO2 were estimated to be 3.68, 230.51, 0.05, 0.36, 0.60 and 0.03 Gg for rice
husk, 33.75, 2140.35, 1.75, 2.91, 6.20 and 0.75 Gg for rice straw, 1.11, 76.28, 0.02, 0.02 and 0.03 Gg for
corncobs and 42.12, 3185.53, 1.22, 4.90, 8.74 and 0.61 Gg for bagasse respectively. Rice straw, however,
had significantly (p < 0.05) higher potential of gaseous pollutant emission factors. Bagasse had the
highest values of total emissions followed by rice straw, rice husk and corncobs. Rice straw and bagasse,
on cumulative basis, contributed more than 90% of total emissions of gaseous pollutants. Results reported
in this study are important in formulating provincial and regional emission budgets of gaseous pollutants
from burning of agricultural residues in Pakistan.
Ó 2013 Elsevier Ltd. All rights reserved.

* Corresponding author. Tel.: þ92 (0) 41 920 1566; fax: þ92 (0) 41 920 0671.
E-mail addresses: [email protected], [email protected] (M.S. Arif).

1352-2310/$ e see front matter Ó 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.atmosenv.2013.11.046
190 M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197

1. Introduction (Shah et al., 1997). Emission factors, measured over longer time
periods, are helpful in making emission inventories to control air
Pakistan, with an annual population growth rate of 2.4% and pollution at local, national and regional levels. Emission factors,
projected population of 18 million people, has been witnessing from different biomass burning, are integral components for mak-
severe energy crisis over the last five years. At present, approxi- ing emission inventories and budgets.
mately 54% of energy requirement is met through fossil fuels such Although studies on emissions from biomass burning are well
as oil and gas, and rest of the energy is obtained from biomass fuel documented across the globe (e.g. Delmas and Servant, 1982;
such as wood and agricultural residues (Tahir et al., 2010). Crop Lacaux et al., 1993) including studies of Saud et al. (2011) in India
residues are value added organic byproducts generated from har- and Zhang et al. (2008) in China, the research area is yet to be
vesting and processing of agricultural crops. explored in Pakistan. It should be noted that there are limited
Due to lack of knowledge regarding the significance of crop emission factors available in developing countries, and those re-
residues, they are often burned in the field (Samra et al., 2003). ported in the literature often varied dramatically due to difference
Agricultural open field burning is widely practiced in the rural areas in fuel properties and combustion conditions. In addition, emission
and suburbs to dispose of biomass waste (Yevich and Logan, 2003). factors measured in the laboratory may differ from those obtained
Several reasons favor burning of crop residue including cleaning in field measurements (Roden et al., 2006, 2009; Shen et al., 2010).
and field preparation, meeting domestic energy requirements, Therefore, there is need to assess emission characteristics of
fertilizing the field with ash and offering the pest control (Huang biomass burning in Pakistan since sever energy crisis have forced
et al., 2012; Korontzi et al., 2006). However, the quantity of the large population to use firewood, crop residues and animal dung for
crop residues burned and the fire intensity strongly influence the meeting energy demands, especially in rural and peri-urban areas.
amount of carbon and nutrients released during the fire (Sharma Keeping in context of the above discussion, a field scale study was
and Mishra, 2001). performed to evaluate the emission characteristics of commonly
Crop residues and/or agricultural wastes are important domes- burned agricultural biomass wastes in Pakistan i.e. rice straw, rice
tic fuels since ancient times. Nearly half of the world population husk, corn cobs and bagasse. Furthermore, to our knowledge, this is
utilizes crop residues for domestic heating and cooking, especially the first study determining emission concentrations, emission fac-
in developing countries (Guoliang et al., 2008). According to esti- tors and emission inventories of trace gases from burning of crop
mates of Andreae and Merlet (2001) and Bond et al. (2004), burning residues in Pakistan. The current study was designed to:
of crop residues accounts for 540 and 475 Tg dry matter combustion
per year respectively. Therefore, air quality deterioration, in cities  investigate the emissions of different gaseous pollutants (CO,
located around major agricultural sectors, is perhaps not surprising CO2, NO2, NO, NOx, SO2) from burning of rice straw, rice husk,
(Cancado et al., 2006). There also have been extensive evidence of corncobs and bagasse.
overlooking the emissions of trace gases from crop residue burning  characterize and compare the emission factors of rice straw, rice
to a large extent, because these fires are often short-lived and do husk, corncobs and bagasse burning
not offer significant time to be detected and quantified under  prepare emission inventories to estimate total emissions of trace
natural conditions (Smith et al., 2007; Vander-Werf et al., 2010). gases
Field and domestic burning of crop residues consist of pyrolysis,
smoldering and flaming processes, however, dominance of these
processes and resultant gas emissions largely depend on the type of 2. Materials and methods
material being burnt (Andreae and Merlet, 2001). For example,
agricultural residues usually follow flaming mode of burning that 2.1. Selection, sampling and preparation of crop residue samples
results in higher NOx concentrations, dung cakes are burnt through
smoldering mode and burning fuel wood normally pass through all Rice straw, rice husk, corncobs and bagasse were used in this
three stages of combustion (Saud et al., 2011). study because they are burnt in the agricultural fields as waste
Environmental problems associated with crop residue burning products and in homes and/or industries for energy in Pakistan.
include smoke, trace gases and particulate matter (Bijay-Singh and Samples of crop residues were collected in triplicate from farmers’
Yadvinder-Singh, 2003). Concentrations of the greenhouse gases fields and agricultural processing industry around Faisalabad and
have increased over the past 50 years as a result of anthropogenic Kasur in Punjab, Pakistan (Fig. 1). Rice straw and bagasse were
activities including agriculture, and have accelerated the rise in collected from Gatwala and corncobs were collected from Jarran-
average global temperature (IPCC, 2001). In particular, uncontrolled wala, suburbs of Faisalabad. However, rice husk samples were ob-
and incomplete open-field burning results in emission of toxic air tained from Kasur. Samples were air dried under outdoor ambient
pollutants and greenhouse gases which affect the atmospheric conditions for several days before the start of experiment. When
chemistry (Andreae and Merlet, 2001; Kanabkaew and Oanh, 2011). uniformly air-dried, samples were kept in sealed plastic bags.
Agricultural crop residue burning is also the prime source of the
micron-sized aerosols which affect the composition of atmosphere 2.2. Construction and design of burning tower
(Awasthi et al., 2011; Saud et al., 2011). Trace gases emitted during
burning, carbon monoxide and nitrogen oxide, are the main pre- For this experiment, a metallic combustion tower was designed
cursors of tropospheric ozone (O3), decreasing the concentrations with an aim to facilitate the analysis by channelizing the smoke
of tropospheric hydroxyl radical (OH) (Mauzerall et al., 1998); the through one stack (Fig. 2). The tower consisted of an inverted
later holds potential threats to environment, ecosystem and human funnel shaped cylindrical bottom having 1.2 m diameter and 1.0 m
health (Cheng et al., 2000). height. A stack with internal diameter of 0.2 m and length of 1.2 m
Emission factor is a crucial parameter used to estimate and was attached at the top end of the cylindrical bottom (Fig. 2a). The
quantify emission of trace gases and aerosols from biomass burning stack was at 1.2 m height from the ground. The cylindrical bottom
which describes compounds or substances emitted per amount of was supported with iron rods to keep it at 0.2 m height from
dry fuel burned (Andreae and Merlet, 2001; Yang et al., 2008). ground level (Fig. 2b). A metallic burning table of 0.4 m  0.4 m
Emission factors of gaseous pollutants vary with time and space, dimension was also constructed using a coarse iron wire-gauze
and also depend on type, quality and composition of biomass fuel which has 0.2 m long legs at its four corners. The stack had an
M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197 191

Fig. 1. Sampling locations of rice husk, rice straw, corncobs and bagasse in Punjab, Pakistan. 1Rice husk, 2Rice straw, 3Bagasse, 4Corncobs.

opening at 0.6 m height from its bottom for insertion of the CO, NO, NO2 and SO2 respectively. The accuracy of the instrument
instrumental probe and recording of different parameters. Keeping for CO, NO, NO2 and SO2 emission concentrations was 5% of the
the burning material on the perforated metallic stand, at 0.2 m measured value.
height, ensured uniform 3-D movement of gases and ample supply
of oxygen to facilitate uniform burning under ambient conditions. 2.3.2. Experimental process
Before each burning test, the selected crop residue was
2.3. Emission analysis weighed and placed on metallic perforated burning table designed
especially to facilitate residue burning (Fig. 3). After ignition,
2.3.1. Principle of flu gas analyzer sampling probe of the analyzer was inserted into the stack to
Trace gas emissions were measured using a digital flu gas measure trace gas concentrations from the start to the end of each
analyzer, testo 350-S (testo AG, Germany) by following a modified burning cycle of residue combustion at 10 s interval (Jenkins et al.,
protocol of Li et al. (2009). The analyzer draws gases from the stack 1996). Experimental conditions and design of the combustion
with the help of sampling probe. Gases pass through the sensors tower allowed natural and uniform ventilation during each
and sensors, based on the principle of selective ion potentiometery, burning event. Time was noted for each burning event and when
measure the electrochemical potential differences. The range of the burning process was completed, ash was collected and weighed to
instrument for emission concentrations of CO2 was 0e50 vol. % calculate percent mass loss. Each crop residue burning test was
whereas range was 0e10000, 0e3000, 0e500 and 0e5000 ppm for repeated three times throughout the experiment; however, where

Fig. 2. Experimental set up: (a) schematic diagram, (b) actual burning tower.
192 M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197

Fig. 3. Air dried biomass on metallic stand before burring: (a) rice husk, (b) rice straw, (c) bagasse, (d) corn cobs.

appropriate, mass weighted means of the data are presented in (ppmv) were measured using the digital flu gas analyzer (testo 350-
tables and figures. S). At the start of the burning cycle, the probe of the analyzer was
inserted into the stack through the designed hole to record the said
2.4. Analytical protocols parameters for each fuel burning event every 10 s until the burning
cycle was complete. Emission concentrations were used to calculate
2.4.1. Moisture content and mass loss emission factors of the gaseous pollutants (Guoliang et al., 2008).
Moisture content was measured gravimetrically by drying crop
residue samples at 90  C for 48 h in a pre-heated oven. Samples 2.5. Calculation of emission factors
were cooled in a desiccator before they were reweighed and
moisture content was calculated on percent dry mass basis. Mass Fuel based emission factors of gaseous pollutants represent
loss was calculated by weighing the fuel samples before and after mass of the specie released per unit fuel weight (Andreae and
the combustion process was completed (ash content). Mass loss Merlet, 2001). Emission factors of gaseous pollutants were calcu-
was also presented on percent mass basis. lated using the mass balance equation described by Jenkins et al.
(1996) and Guoliang et al. (2008) and were expressed on g per kg
2.4.2. Total carbon (C), nitrogen (N) and sulfur (S) contents of dry weight of the fuel:
biomass
Oven-dried crop residue samples from moisture content deter- Ztf
103 wi
mination were further used for the measurements of total C, N and Ei ¼ As uCi dt (1)
mfd 22:4
S contents. For C and N analysis, the oven-dried samples were t0
ground using a ball mill (Retsch MM301) to homogenize the sam-
ples prior to analysis on a Carlo Erba Na 1500 CNS analyzer (Thermo Where
Fisher Scientific, Waltham, MA). C and N content of the samples
were calibrated using the standards atropine and acetanilide and Ei ¼ Emission factor for species i
an internal reference sample. For S analysis, 100 mg residue ma- mfd ¼ Mass of crop residue used in the each burning test
terial was digested under high pressure with nitric acid and t0 ¼ Initial start time for each burning test
hydrogen peroxide in sealed Teflon vessels using a Milestone tf ¼ Finishing time for the test
destruction microwave oven (MLS 1200 mega). After digestion, the As ¼ Stack area (0.03 m2)
samples were analyzed for S contents on an inductively-coupled u ¼ Average stack gas velocity
plasma emission spectrophotometer (ICP, Spectroflame Flame Ci ¼ Sample concentration of species i, and
VML2). Standard reference solutions for S were analyzed for cali- wi ¼ Molecular weight of species i
bration on ICP. C, N and S contents of residue samples were
expressed on percent dry mass basis.
2.6. Quantification of crop residue production and burning in
2.4.3. Stack gas velocity, flu temperature, burning cycle and Pakistan
emission concentrations of gaseous pollutants
The stack gas velocity (m s1), flu temperature ( C), burning cycle Crop residues production was estimated from crop production
(s) and emission concentrations of CO, CO2, NO2, NO, NOx and SO2 data (Government of Pakistan, 2011e12) and relevant residue
M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197 193

generation rate or ratio (Singh and Gu, 2010) using following treatment effects were found. However, where appropriate, figures
relationship: and tables contain means of three replicates.

Crop residues ðMtÞ ¼ Crop production ðMtÞ 3. Results and discussion


 crop to residue ratio (2)
3.1. Biomass characteristics
Total amount of residue burnt, for each residue, was quantified
as under: Physical and chemical characteristics of rice husk, rice straw,
corncobs and bagasse are summarized in Table 1. Moisture content
Total residue burnt ðMtÞ ¼ Total crop residue ðMtÞ
ranged from 9.74  0.43% for rice husk to 12.06  0.18% for bagasse.
 Residue dry matter fraction Mass loss percent values were 85.66  0.17% for rice husk,
 Crop residue burnt ð%Þ 81.07  0.07% for rice straw, 97.06  0.04% for corncobs and
89.59  0.62% for bagasse. Mass loss percent of corncobs was
(3) significantly (p < 0.05) higher compared to that from rice husk, rice
Dry matter fraction for each crop residue was obtained from straw and bagasse.
Streets et al. (2003) and crop residue percent being burnt was C, N and S contents of crop residues are also shown in Table 1. C
estimated to be 25% for each crop residue (Iqbal and Goheer, 2008). contents of corncobs and bagasse were 44.70  0.04 and
43.87  0.10% respectively which were significantly (p < 0.05)
higher than C content of rice husk (36.29  1.60%) and rice straw
2.7. Estimation of total annual trace gases emissions
(39.16  0.05%). N contents were 0.47  0.03% for rice husk,
0.59  0.04% for rice straw, 0.44  0.03% for corncobs and
Total annual emission of each gaseous pollutant from burning of
0.62  0.02% for bagasse. S contents of rice straw, 0.17  0.01%, were
biomass fuel was calculated using following relationship described
the highest among the crop residue used in this study and were
by Kanabkaew and Oanh (2011) and Yang et al. (2008):
significantly (p < 0.05) different from rice husk, corncobs and
Total annul emissions ¼ M  EF (4) bagasse.
The moisture content, mass loss, C, N and S contents of biomass
Where, fuel have a significant impact on the burning and emission char-
acteristics of biomass. In our study, bagasse had the highest mois-
E ¼ Total annual emission (Gg) ture contents compared to rice husk, rice straw and corncobs. The
M ¼ Quantity of crop residues burnt in a year (Mt dry mass of moisture content of rice straw (11.05%) was in accordance with the
residue) range of moisture content (10e12%) for rice straw previously re-
EF ¼ Emission factors of gaseous species (g kg1 fuel dry mass) ported by Buzarovska et al. (2008). However, the moisture content
of the rice husk was higher compared to that 7.20% observed by
Ileleji and Zhou (2008). This higher moisture content of rice husk
2.8. Modified combustion efficiency (MCE) could be attributed to regional climatic conditions. The results of
mass oxidized (mass loss) for bagasse was similar to those reported
Ward et al. (1992) described combustion efficiency (CE) as the by Sahai et al. (2011). However, mass loss values for rice straw, rice
ratio of carbon released as CO2 to the total mass of carbon in the fuel husk and corncobs was found to be 81.07, 85.66 and 89.59% which
biomass. CE may be considered helpful in determination of the differed slightly from the reported 90% value of mass loss for these
completeness of the combustion as well as indication of process crop residues (Sahai et al., 2011). In this study, we have also re-
and/or processes dominant during the combustion. CE is usually ported C, N and S contents of crop residues since the chemical
measured as under: composition of the crop residue is an important factor in deter-
mining the emission factors of gaseous pollutants as argued by
CE ¼ CCO2 =CTotal Zhang et al. (2008).

Where CCO2 is the carbon emitted in CO2 form and CTotal is the total 3.2. Burning characteristics
amount of carbon in gaseous and particulate emissions. In the
current study, CCO2 and CCO were measured but particulate matter Flu temperature, stack gas velocity, burning cycle and modified
contents were not measured; hence, the modified combustion ef- combustion efficiency (MCE) for rice husk, rice straw, corncobs and
ficiency (MCE) was calculated following relationship proposed by bagasse are presented in Table 2. Flu temperatures of rice straw
Zhang et al. (2008):
 
MCE ¼ CCO2 = CCO2 þ CCO (5)
Table 1
Moisture content, mass loss, total carbon, total nitrogen and total sulfur content of
rice husk, rice straw, corncobs and bagasse.

2.9. Statistical analysis Parameter Rice husk Rice straw Corncobs Bagasse

Moisture 9.74 (0.43) a 11.05 (0.27) ab 11.43 (0.28) a 12.06 (0.18) a


Data regarding moisture content (%), mass loss (%), C (%), N (%), S content (%)
(%), flu temperature ( C), stack gas velocity (m s1), burning cycle Mass loss (%) 85.66 (0.17) c 81.07 (0.07) d 97.06 (0.04) a 89.59 (0.62) b
Total carbon (%) 36.29 (1.60) b 39.16 (0.05) b 44.70 (0.04) a 43.87 (0.10) a
(s), gaseous pollutant emission concentration (ppmv) and gaseous Total nitrogen (%) 0.47 (0.03) bc 0.59 (0.04) ab 0.44 (0.03) c 0.62 (0.02) a
emission pollutant factors (g kg1), measured and/or calculated on Total sulfur (%) 0.06 (0.00) b 0.17 (0.01) a 0.03 (0.00) c 0.07 (0.00) b
replicate samples, were subjected to one way analysis of variance Values are means of three replicates. Standard errors of means are enclosed in
(ANOVA). Tukey’s HSD postdoc test was used for multiple means parenthesis. In a row, for specified parameter, means with different letters differ
comparisons technique only for those parameters where significant significantly from each other at p < 0.05.
194 M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197

(245.50  6.16  C) and bagasse (263.50  5.01  C) were significantly 1.44  0.01 g kg1 respectively (Fig. 4d); they were significantly
higher (p < 0.05) compared to that for rice husk (115  2.31  C) and (p < 0.05) higher from NO emission factors of corncobs
corncobs (197.57  2.72  C). Values of stack gas velocity were (0.70  0.01 g kg1). Emission factors of NOx ranged from
12.33  0.10, 14.34  0.91, 14.17  0.29 and 18.39  0.30 m s1 for 1.23  0.01 g kg1 for corncobs to 3.16  0.08 g kg1 for rice straw
rice husk, rice straw, corncobs and bagasse respectively. Bagasse (Fig. 4e). Emission factors of SO2 were 0.11  0.03, 0.38  0.03,
had significantly (p < 0.05) higher stack gas velocity values 0.02  0.00 and 0.18  0.02 g kg1 from burning of rice husk, rice
compared to rice husk, rice straw and corncobs. There were sig- straw, corncobs and bagasse respectively (Fig. 4f). Emission factors
nificant (p < 0.05) differences in length of burning cycle for rice of SO2 from rice straw were found to be highest and significantly
husk, rice straw, corn cobs and bagasse. MCE ranged from 0.976 for (p < 0.05) different from rice husk, corncobs and bagasse.
rice husk and rice straw to 0.980 for bagasse. Bagasse had signifi- Emission factor is an important tool to estimate total gaseous
cantly (p < 0.05) higher MCE compared to rice husk, rice straw and pollutant emissions to help making pollution inventories and pol-
corncobs. icy decision to mitigate air pollution (van Leeuwen and Hermens,
In this study, stack gas velocity was measured under ambient 1995; Andreae and Merlet, 2001; Yang et al., 2008). Emission fac-
conditions since it determines speed of gaseous pollutant emis- tors for different crop residues have been widely reported in liter-
sions from open burning of residue biomass and depends on the ature, especially of rice straw. The rice straw produced the highest
ambient environmental conditions like air flow to ensure optimum emission factors of the trace gases in the current study. The emis-
oxygen concentrations for complete and efficient burning sion factors of CO, CO2, NO2, NO, NOx and SO2 from rice straw were
(Wardoyo et al., 2006). Bagasse showed the highest value of stack calculated to be 17.19  0.28, 1090.1  24.0, 0.89  0.03, 1.48  0.04,
gas velocity in this study. Burning cycle could also serve as 3.16  0.08 and 0.38  0.03 g kg1 respectively which showed
important determinant of combustion efficiency of biomass and considerable agreement with data of some previous studies on rice
depends on physical and chemical characteristics of fuel biomass straw e.g. emission factors of CO2 101 g kg1 (Smith et al., 1993),
(Ward et al., 1992). MCE was measured to distinguish between NOx 3.43 g kg1 (Guoliang et al., 2008) and NO2 0.79 g kg1 (Zhang
flaming and smoldering mode of combustion during crop residue et al., 2008). However, emission factors of CO and SO2 were found to
burning. MCE in our study was 0.976, 0.976, 0.978 and 0.980 for rice be different than those reported in literature e.g. Jenkins et al.
husk, rice straw, corncobs and bagasse respectively which falls in (1996) reported 31.41 and 0.62 g kg1 emission factors of CO and
the range of 0.9e1.0 suggested by Reid et al. (2005) for fires SO2 respectively which were higher than those reported in our
following flaming as dominant mode of combustions. However, it is study. The emission factors of CO, CO2, NO2, NO, NOx and SO2 from
also an established fact that smoldering and flaming mode of bagasse were 12.39  0.08, 937.03  9.07, 0.36  0.03, 1.44  0.02,
combustions cannot be separated completely when biomass is 2.57  0.04, and 0.18  0.02 g kg1 respectively. Emission factors of
burnt under field conditions. Nevertheless, MCE of crop residues in NOx and NO for bagasse from this study were comparable to
our study support the well-documented claim that agricultural 2.6 g kg1 NOx (Dennis et al., 2002) and 1.7 g kg1 NO (Brocard et al.,
crop residue burn under flaming mode under field and laboratory 1996). However, emission factors of CO, CO2, NO2 and SO2 from
conditions (Saud et al., 2011; Zhang et al., 2008). bagasse were lower from those previously reported e.g. CO
34.7 g kg1 and CO2 1130 g kg1 (Kanabkaew and Oanh, 2011), NO2
3.3. Emission factors of gaseous pollutants 1.6 g kg1 (Brocard et al., 1996), SO2 0.23 g kg1 (Kato, 1996) and
0.50 g kg1 (Gadi et al., 2003). These differences in emission factors
Emission factors (EFs) of gaseous pollutants, calculated from could be due to factors like moisture content and local climatic
emission concentrations, of rice husk, rice straw, corncobs and conditions (Goldammer et al., 2009), physical and chemical differ-
bagasse are shown in Fig. 4. The mean emission factors of CO2 for ences in the crop residue composition of different regions (Lobert
rice husk, rice straw, corncobs and bagasse were 880.48  8.99, and Warnatz, 1993) and, especially N contents for the variations
1090.1  24.0, 595.44  10.4 and 937.03  9.07 g kg1 respectively in NOx emission factors (Zhang et al., 2008).
(Fig. 4a). Emission factor of CO2 of rice straw were significantly The emission factors from corncobs and rice husk have not
(p < 0.05) higher compared to rice husk, corncobs and bagasse. widely been reported in the literature and this is perhaps the first
Emission factors of CO from rice husk (14.04  0.18 g kg1), rice attempt in this regard. The emission factors of CO, CO2, NO2, NO,
straw (17.19  0.28 g kg1), corncobs (14.04  0.18 g kg1) and NOx and SO2 from burning of corncobs were observed to be
bagasse (12.39  0.08 g kg1) followed order similar to that of CO2 8.63  0.12, 595.44  10.38, 0.16  0.01, 0.70  0.01, 1.23  0.02 and
emission factors (Fig. 4b). Emissions factors of NO2 were 0.02  0.00 g kg1 respectively. The results of emission factors of
0.19  0.03, 0.89  0.03, 0.16  0.01 and 0.36  0.03 g kg1 for rice SO2 and NOx were in reasonable agreement with 0.04 g kg1 for SO2
husk, rice straw, corncobs and bagasse respectively (Fig. 4c). by Cao et al. (2008) and 1.27 g kg1 for NOx by Zhang et al. (2008)
Emission factors of NO2 from rice straw were significantly which were based on the burning of aggregated maize crop waste.
(p < 0.05) higher compared to that from rice husk, rice straw, However, the emission factors of CO and CO2 from our study for
corncobs and bagasse. Emission factors of NO from rich husk, rice corncobs differed from those reported by Andreae and Merlet
straw and bagasse were 1.38  0.02, 1.48  0.04 and (2001) for CO (53 g kg1) and Zhang et al. (2008) for CO2

Table 2
Flu temperature, stack gas velocity, burning cycle and modified combustion efficiency (MCE) of rice husk, rice straw, corncobs and bagasse.

Parameter Rice husk Rice straw Corncobs Bagasse

Flu temperature ( C) 115 (2.31) c 245.50 (6.16) a 197.57 (2.72) b 263.50 (5.01) a
Stack cas velocity 12.33 (0.10) c 14.34 (0.91) b 14.17 (0.29) b 18.39 (0.30) a
(m s1)
Burning cycle (s) 953.33 (5.24) b 990 (4.04) a 618.33 (4.91) d 783.33 (8.25) c
Modified combustion 0.976 (0.00) a 0.976 (0.00) a 0.978 (0.00) b 0.980 (0.00) c
efficiency (MCE)

Values are means of three replicates. Standard errors of means are enclosed in parenthesis. In a row, for specified parameter, means with different letters differ
significantly from each other at p < 0.05.
M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197 195

20
1200
a
18 a a b
1000 b
16 b

CO (g kg -1 )

CO 2 (g kg -1 )
b 800
14
c c
12 600

10 400
d
8
200
6
0
Rice husk Rice straw Corncobs Bagasse Rice husk Rice straw Corncobs Bagasse

1.0
a
c 1.6
d a
a a
0.8 1.4
NO 2 (g kg -1 )

1.2

NO (g kg -1)
0.6 1.0

0.8 b
b
0.4
0.6
c 0.4
0.2 c
0.2

0.0 0.0
Rice husk Rice straw Corncobs Bagasse Rice husk Rice straw Corncobs Bagasse

3.5 0.5
a
3.0
e f a
b 0.4
2.5 c
NO x (g kg -1 )

SO 2 (g kg -1 )

2.0 0.3

1.5
d b
0.2
b
1.0
0.1
0.5
c
0.0 0.0
Rice husk Rice straw Corncobs Bagasse Rice husk Rice straw Corncobs Bagasse

Fig. 4. Gaseous pollutant emission factors from burning of rice husk, rice straw, corncobs and bagasse: (a) CO, (b) CO2, (c) SO2, (d) NOx, (e) NO2, (f) NO (units: g kg1). Values are
average of three replicates. Error bars are standard error of means (n ¼ 3). Bars with different letters differ significantly from each other at p < 0.05.

(1160 g kg1). This difference could be due to the reason that they Iqbal and Goheer, 2008), total crop residue burned for rice husk,
measured emission factors by burning aggregate maize crop res- rice straw, corncobs and bagasse was found to be 262, 1964, 128 and
idue; however, in contrast, we used corncobs which could result in 3400 Mt respectively (Table 4). Bagasse had the highest values for
different emission factors through changes in the composition of residue production and combustion followed by rice straw, rice
biomass (Lobert and Warnatz, 1993). The emission factors of CO, husk and corncobs respectively.
CO2, NO2, NO, NOx and SO2 from burning of rice husk were Total emissions (Gg) from crop residues for CO, CO2, NO2, NO,
14.04  0.18, 880.48  8.99, 0.19  0.01, 1.38  0.02, 2.31  0.04 and NOx and SO2 are presented in Table 5. Total emissions from bagasse
0.11  0.03 g kg1 respectively. The results suggested considerable were 42.12, 3185.53, 1.22, 4.90, 8.74 and 0.61 Gg for CO, CO2, NO2,
differences in emission factors of rice straw and rice husk due to the
very fact that they were sampled from different locations.
Table 3
Estimation of production of rice straw, rice husk, bagasse and corncobs in Pakistan in
3.4. Emission estimates, inventories and allocation of gaseous 2011e12.
pollutants
Residue type Crop Crop to Total crop residue
production (Mt)a residue ratiob production (Mt)c
Rice husk, rice straw, corncobs and bagasse are important res-
Rice husk 6160 0.20 1232
idue producing crops being used as biomass fuel in Pakistan. In
Rice straw 6160 1.50 9240
order to prepare emission estimates, inventories and allocations, Corncobs 4271 0.30 1281
quantity of crop residues was estimated to be 1232, 9240, 1281 and Bagasse 58,038 0.33 19,153
19153 Mt for rice husk, rice straw, corncobs and bagasse respec- a
Government of Pakistan (2011e12).
tively (Table 3). Based on the dry matter fraction (Streets et al., b
Singh and Gu (2010).
c
2003) and percent of the crop residues being combusted (25%; Metric tons.
196 M. Irfan et al. / Atmospheric Environment 84 (2014) 189e197

Table 4 We have reported emission factors and total emissions from


Estimation of residue burnt in Pakistan in 2011e2012. combustion of crop residues which are commonly used in indus-
Residue type Total crop Dry matter Crop residue/dry Total residue trial and household sectors of Pakistan. According to best of our
residue (Mt) fractiona matter burnt (%)b burnt (Mt)c knowledge, this is the first study reporting emission inventories of
Rice husk 1232 0.85 25 262 gaseous pollutants from burning of agricultural residues. Results
Rice straw 9240 0.85 25 1964 described in the study are assumed to be helpful in making national
Corncobs 1281 0.40 25 128 and provincial estimates of gaseous pollutants from frequently
Bagasse 19,153 0.71 25 3400
consumed agricultural residue biomass. However, it should be
a
Streets et al. (2003). noted that variations in fuel properties and combustion conditions
b
Iqbal and Goheer (2008).
c
could lead to rather rough estimates of emission factors with high
Metric tonns.
degree of uncertainty.

NO, NOx and SO2 respectively. Total emissions from bagasse for CO, 4. Conclusions and future research
CO2, NO and NOx were the highest compared to those from rice
straw, rice husk and corncobs. However, total emissions of NO2 Recent energy crisis has led to increased dependency on
(1.75 Gg) and SO2 (0.75 Gg) from the rice straw were found to be agriculture-based biomass fuel combustion in agro-industrial and
highest compare to the other crop residues (Table 5). Total emis- household sectors in Pakistan. Rice husk, rice straw, corncobs and
sions for each gaseous pollutant from burning of crop residue were bagasse represent common biomass fuels in Pakistan. Biomass fuels
80.66 Gg for CO, 5632.67 Gg for CO2, 3.04 Gg for NO2, 8.19 Gg for NO, differed markedly for physical, chemical and combustion charac-
15.70 Gg for NOx and 1.42 Gg for SO2. Calculated from Table 5, teristics. Modified combustion efficiency (MCE) ranged from 0.976
emission allocations for gaseous pollutants from rice husk and to 0.980 indicating flaming as the mode of combustion under
bagasse together accounted for 94.1, 94.6, 97.7, 95.4, 95.2 and 95.8% ambient conditions. This study reports experimentally measured
total emission of CO, CO2, NO2, NO, NOx and SO2. Our study also gaseous pollutant emission concentrations, emission factors and
showed that the cumulative contribution of rice husk and corncobs emission inventories of rice husk, rice straw, corncobs and bagasse
to the total emissions of gaseous pollutants was marginal. combusted under ambient outdoor conditions using specially
Total emissions of gaseous pollutants from burning of rice husk, designed burning tower. Emission factors of CO, CO2, NO2, NO, NOx
rice straw, corncobs and bagasse were many fold lowered and SO2 were determined to be 14.05  0.18, 880.48  8.99,
compared to those reported in studies from China (Zhang et al., 0.19  0.01, 1.38  0.02, 2.31  0.04 and 0.11  0.03 g kg1 for rice
2008) and India (Saud et al., 2011). However, China and India are husk, 17.19  0.28, 1090.07  24.0, 0.89  0.03, 1.48  0.04,
the largest countries of the world with remarkably higher agri- 3.16  0.08 and 0.38  0.03 g kg1 for rice straw, 8.63  0.12,
cultural crop production and crop residue generation. We esti- 595.44  10.38, 0.16  0.01, 0.70  0.01, 1.23  0.02 and
mated total emissions of gaseous pollutants considering burning of 0.02  0.00 g kg1 for corncobs and 12.39  0.08, 937.03  9.07,
only 25% crop residue as is the case in China suggested by Gao et al. 0.36  0.03, 1.44  0.02, 2.57  0.04 and 0.18  0.02 g kg1 for
(2002) and Iqbal and Goheer (2008); however, recent energy crisis bagasse. Results of emission factors of gaseous pollutants from
in Pakistan has led to far higher utilization of crop residues as burning of rice husk, rice straw, corncobs and bagasse were in
biofuel which may mean that actual total emission could be higher. reasonable agreement with those reported elsewhere. Total emis-
We have observed that bagasse contributed largely to the budgets sions of CO, CO2, NO2, NO, NOx and SO2 from burning of biomass
of gaseous pollutants especially of CO, CO2 and NOx in Pakistan. This fuels were estimated to be 80.66, 5632.67, 3.04, 8.19, 15.70 and
could be related to the considerably higher emission factors and the 1.42 Gg respectively. On cumulative basis, rice straw and bagasse
most importantly, larger amounts of bagasse production as contributed more than 90% of total emissions of gaseous pollutants.
compared to rice straw, rice husk and corncobs. The rice straw and Results of this study are important in formulating provincial and
the bagasse contributed more than 90% of total emission of gaseous regional budgets of gaseous pollutants from burning of agricultural
pollutants. Field burning of rice husk, rice straw, corncobs and residues. However, biomass fuels like cotton sticks and dung cake
bagasse is not commonly practiced in Pakistan; however, these needs to be assessed for their role in emission of gaseous pollutants
crop residue are largely consumed in industrial and rural sectors. In in future since they also represent important biofuels in rural sec-
addition, household income of large percent of farmers in Pakistan tors of Pakistan.
is low whereas energy supply and cost is becoming expensive so
they usually opt to use crop residues to meet domestic energy re-
Appendix A. Supplementary data
quirements. The latter claim is supported by studies of Cao et al.
(2008) and Chen (2001) who found that field burning of crop res-
Supplementary data related to this article can be found at http://
idues was related to income level of farmers.
dx.doi.org/10.1016/j.atmosenv.2013.11.046

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