Modified Combustion Efficiency

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Atmospheric Environment 42 (2008) 8432–8441

Contents lists available at ScienceDirect

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

A laboratory study of agricultural crop residue combustion in


China: Emission factors and emission inventory
Hefeng Zhang a, Xingnan Ye a, Tiantao Cheng a, Jianmin Chen a, *, Xin Yang a, *,
Lin Wang b, Renyi Zhang b
a
Center of Atmospheric Chemistry Studies, Department of Environmental Science and Engineering, Fudan University, Handan Road 220, Shanghai 200433, China
b
Department of Atmospheric Science, Texas A&M University, College Station, TX 77843, USA

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

Article history: The burning of agricultural crop residue represents a major source of trace gases (CO, CO2,
Received 9 May 2008 NO, NO2, and NOx) and particulate matter on a regional and global scale. This study
Received in revised form 11 August 2008 investigates the gaseous and particulate emissions from the burning of rice, wheat and
Accepted 11 August 2008
corn straws, which are three major agricultural crop residues in China, using a self-built
burning stove and an aerosol chamber. Emission factors of CO2, CO, NO, NO2 and NOx were
Keywords:
measured to be 791.3, 64.2, 1.02, 0.79 and 1.81 g kg1 for rice straw, 1557.9, 141.2, 0.79, 0.32
Agricultural crop residue
and 1.12 g kg1 for wheat straw, and 1261.5, 114.7, 0.85, 0.43 and 1.28 g kg1 for corn straw,
Gaseous pollutant
Emission factor respectively. The corresponding emission factors of particle number are 1.8  1013,
Emission inventory 1.0  1013, and 1.7  1013 particles kg1, respectively. The total emissions of CO, CO2, and
Emission allocation NOx from rice, wheat and corn straw burnings in China for the year 2004 were estimated to
be 22.59, 252.92, and 0.28 Tg, respectively. The percentages of CO, CO2, and NOx to the total
emissions were 13.9%, 15.3%, and 31.4% for rice straw, 32.9%, 32.5%, and 20.9% for wheat
straw, and 53.2%, 52.2%, and 47.6% for corn straw, respectively. In addition, the emission
allocations of agricultural crop residue burning were also plotted in different regions of
China using a simple geographic information system (GIS).
Ó 2008 Elsevier Ltd. All rights reserved.

1. Introduction global atmospheric chemistry and global climate change


(Levine et al., 1995; Andreae and Merlet, 2001). Active trace
China has a large rural population whose major energy gases emitted from biofuel burning, such as carbon
source has been biofuel (crop residue) for the last two monoxide (CO) and nitrogen oxide (NOx), are precursors of
decades. However, the rapid economic development has tropospheric ozone (O3) that reduce the tropospheric
increased the consumption of commercial energy in rural concentration of the extremely reactive hydroxyl radical
areas. As a result, not being used for domestic energy, more (OH) (Logan et al., 1981; Mauzerall et al., 1998), which
agricultural residues have been directly burned in the field, possesses a greater threat to human health.
especially in grain-producing regions with low population Trace gas emissions from the burning of agricultural
densities, industrially developed regions, and fossil- crop residue in China, including domestic and field burning,
producing regions (Cao et al., 2006). The burning of crop were previously studied by Zhuang et al. (1996). A more
residue has also been considered as an important source of complete estimate of trace gas and aerosol emissions from
atmospheric trace species with significant impacts on biomass burning in China, including biofuel combustion,
field burning of agricultural crop residue, and forest and
grassland fires, has been summarized in detail (Streets
* Corresponding authors. Tel.: þ86 21 6564 2521; fax: þ86 21 6564
2080.
et al., 2003). The contribution of biomass burning to the
E-mail addresses: jmchen@fudan.edu.cn (J. Chen), yangxin@fudan. total emissions of atmospheric trace species in China,
edu.cn (X. Yang). including forest and grassland fires, fuel wood consumption,

1352-2310/$ – see front matter Ó 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2008.08.015
H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441 8433

and the burning of agricultural crop residue, was assessed supplementary instruments to clean, dry and remove static
by Yan et al. (2006) using statistical data, survey data, before particles and gases were injected and dispersed into
expert estimates and a satellite data set. In addition, a few the chamber. All technical properties of AC-FU were
other estimates of emissions from the open burning of completely tested and characterized before the campaign.
agricultural crop residue in China have been studied, for
example, CO (Palmer et al., 2003; Pétron et al., 2004), black 2.2. Experiment process
carbon (BC) and organic carbon (OC) emissions (Cao et al.,
2006), particulate emissions (Li et al., 2007), and emission Rice, wheat and corn straws were chosen as represen-
impacts (Cheng et al., 2000), etc. However, because of the tatives of agricultural crop residue. The rice straw was
difficulty of isolating gaseous pollutants and reducing collected from a rural field in the suburbs of Shanghai, and
uncertainties concerning in domestic and field burning the wheat and corn straws were from a rural region in Hebei
(Li et al., 2007; Sahai et al., 2007), chamber studies can provide province, China. Agricultural crop straw was weighed before
the possibility of a precise understanding of such processes. and after each burning, and the unburned fraction and ash
Emission inventories and emission allocations of trace were collected for weighing with an analytical balance
species are important for model application and analysis. (Sartorius BP211D, resolving ability 10 mg). Before each
Detailed emission inventories of BC and OC from China in burning, the chamber was purged by scrubbing and blowing
the year 2000 were presented by Cao et al. (2006), air and then vacuumed to below 100 Pa. The agricultural
including gridded emissions at 0.2  0.2 resolution. The crop straw was ignited with a propane torch in the stove. The
emissions from a broader level inventory to finely gridded processes of burning could be observed through the glass
emission values may be distributed using Geographic window of the stove. Then, the smoke produced was
Information System (GIS) (USEPA, 1998). Streets et al. introduced into the chamber immediately by turning on the
(2003) used GIS for gridding emissions for several gaseous controlling valve until the pressure between the inside and
pollutants over the Indian and East Asian regions and the outside was equal. Gaseous pollutants were sampled
provided some useful information on a broader scale. In every 15 min for analysis. In the experimental processes,
China, Cao et al. (2005) reported gridding emissions of NOx ambient air was introduced into the chamber through an
from biomass burning for the year 2000. However, little activated charcoal filter and a filter, to maintain the pressure
work has been done on the emission inventories and equilibrium in the chamber.
emission allocations of gaseous pollutants (such as CO, CO2,
and NOx) from the burning of agricultural crop residue 2.3. Sampling instruments
(rice, wheat and corn straws) in China.
This paper reports on a laboratory program for the Chemiluminescence NO–NO2–NOx analyzer (Model 42i,
systematic study of the emission characteristics of rice, Thermo Environmental Instrumental Inc.) was used to
wheat and corn straw burnings in China that has been measure NO, NO2, and NOx concentrations. Particle number
performed in the Aerosol Chamber of Fudan University (AC- concentrations were determined using a condensation
FU) in Shanghai. The emission factor, emission inventory particle counter (CPC) (model 3771, TSI.). CO and CO2 were
and emission allocation of gaseous pollutants from the analyzed by a gas chromatograph (GC930, Shanghai Hai Xin
burning of rice, wheat and corn straws are discussed, Gas Chromatograph Instrument CO., LTD) equipped with
respectively. The concentrations and emission factors of a flame ionization detector and a Ni–hydrogen converter
particle number (PN) are also presented. where both CO and CO2 were converted into CH4.

2. Experimental section 2.4. CO and CO2 standard curve preparation

2.1. Experimental system The CO and CO2 calibration curves were made by inject-
ing standard CO and CO2 gases into a gas chromatograph.
The experimental system consisted of a self-designed Before calibration, 2 ml CO standard gas was diluted with
combustion stove and a stainless-steel environmental aero- Argon gas to a final volume of 500 ml. The amounts of CO2
sol chamber at Fudan University (AC-FU) of 4.5 m3 (Fig. 1), used for calibration were 20, 40, 60, 80, 100, 200, 400, 600,
equipped with a set of analytical instruments. The diameter 800, and 1000 ml, while the diluted CO were 10, 20, 40, 60, 80,
of the combustion stove was 60 cm and its height was 80 cm. 100, 150, 200 ml, separately. Each injected gas volume and
Air was introduced into the combustion stove through a port the corresponding peak area produced by the gas injection
on the bottom. The top of the stove was connected to the were recorded simultaneously, to allow one to determine
aerosol chamber through a stainless steel tube (diameter the equations of the calibration curves. Both CO and CO2
16 mm). AC-FU was able to control temperature from 203 K calibration curves were linear with R2 values exceeding 0.99.
to 373 K and pressure from 14 Pa to 0.22 MPa. Its inner-wall
was plated by a PTFE-Teflon layer of about 0.3 mm in thick- 2.5. Emission factor (EF), combustion efficiency (CE)
ness. The chamber was easily cleaned up by gas-blowing and and emission ratio (ER)
other methods through a manhole. A hygroclip monitor
(model IM-4, Rotronic) was used to measure the temperature Emission factors (EFs) of gaseous pollutants were calcu-
and relative humidity (RH) inside the chamber. A mixing lated by dividing the mass of emission by the mass of the fuel
fan was installed at the bottom of the chamber to give consumed, and expressed as grams of emission per kilograms
the air in the chamber full mixture. Moreover, AC-FU had of consumed fuel (g kg1). The fundamental definition of the
8434 H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441

Fig. 1. Schematic graph of the experiment system: (a) burning stove, (b) aerosol chamber and associated instruments.

fuel-based emission factor is the mass of released compound carbon oxidization during the combustion of biomass fuels
per unit mass of consumed fuel (Andreae and Merlet, 2001) and may be given by the quantified equation:
which is described by the following equation:
CE ¼ C½CO2  =C½total (3)
EFi ¼ Mi =Mfuel (1)
where C½CO2  is the fraction of emitted carbon in form of CO2;
where EFi is the emission factor of species i; Mfuel is mass of C[total] represents the total carbon of gaseous and particu-
burned fuel; Mi is mass of emitted species i. late emissions.
Particle number emission factors were calculated using Emission ratio (ER) relative to CO2 is determined by dividing
the following equation: the excess mixing ratio above the ambient background level by
the excess mixing ratio of simultaneously measured CO2.
EF ¼ Cav V=m (2)
1
where EF is the emission factor (particles kg ); Cav is the 3. Results and discussion
average particle number concentration (particles cm3); V
is the chamber volume (cm3); m is the burned mass (kg). 3.1. Emission factors of gaseous pollutants and particle
Combustion efficiency (CE) is defined as the ratio of numbers
released carbon in the form of CO2 to the total mass of
carbon released during combustion (Ward et al., 1992). It Emission factors (EFs) of gaseous pollutants emitted
may be used to determine the completeness of released from the burning of rice, wheat and corn straws are shown
H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441 8435

in Table 1. For each kind of straw, four burning tests were 2000 3.2
rice straw wheat straw corn straw

CO, CO2 emission factors


conducted successively. About 20 g of straw was burned for 1800 2.8

emission factors (g/kg)


each experiment. 1600

NO, NO2 and NOx


2.4
The average emission factors of CO2 from four tests were 1400
calculated to be 791.3  12.5 (rice straw), 1557.9  85.8 1200 2.0

(g/kg)
(wheat straw), and 1261.5  59.9 g kg1 (corn straw), the 1000 1.6
CO EFs were 64.2  4.9 (rice straw), 141.2  14.8 (wheat 800 1.2
straw), and 114.7  12.4 g kg1 (corn straw), while the NOx 600
0.8
were 1.81  0.09 (rice straw), 1.12  0.19 (wheat straw), and 400
1.28  0.04 g kg1 (corn straw), respectively. For NO and 200 0.4
NO2, NO EFs of rice straw (1.02  0.03 g kg1), wheat straw 0 0.0
CO CO2 NO NO2 NOx
(0.79  0.13 g kg1) and corn straw (0.85  0.06 g kg1)
were significantly higher than NO2 EFs of rice straw Fig. 2. A comparison of gaseous pollutant emission factors from burning of
(0.79  0.05 g kg1), wheat straw (0.32  0.06 g kg1) and rice, wheat and corn straws.
corn straw (0.43  0.03 g kg1), respectively. Emission
factors of CO2 in our study were comparable to the EFs and rice straws. Moreover, the physical properties of crop
reported in the literature (de Zarate et al., 2000; Zhang residue, such as densities and moisture content, could
et al., 2000; Andreae and Merlet, 2001; Air Sciences Inc., affect burning conditions, which could further affect the
2003a,b; Sahai et al., 2007; Li et al., 2007). Emission factors emission factors of gaseous pollutants.
of CO were also in reasonable agreement with the pub- Particle number concentrations and particle number
lished values (Zhang et al., 2000; Andreae and Merlet, emission factors from rice, wheat and corn straw
2001; Dhammapala et al., 2006; Li et al., 2007). However, burnings are shown in Table 2. The particle number
emission factors of NOx in our study were lower than those concentrations were (7.3  0.3)  104, (3.9  0.7)  104, and
from other reported biomass burnings such as wheat straw (7.5  0.6)  104 particles cm3 for rice, wheat, and corn
(2.63 g kg1, 1.70  1.68 g kg1) (Dennis et al., 2002; Sahai straws, respectively. It may be noticed that wheat straw
et al., 2007), agricultural residues (2.5  1.0 g kg1) burning produced lower particle number concentration
(Andreae and Merlet, 2001), and wheat straw and corn than rice and corn straw burnings. There is little data on
straw (3.3  1.7 g kg1, 4.3  1.8 g kg1) (Li et al., 2007). This particle number concentrations of agricultural crop residue
could probably be explained by the fact that NOx emissions burning. Considering the similarity between agricultural
were related to the N content and/or physical properties of fires and wood fires, we compared our results with
crop residue. previous studies on wood fires. The particle number
Comparison of gaseous pollutant emission factors from concentrations of rice, corn and wheat straw burnings in
the burning of rice, wheat and corn straws is presented in our study were comparable with the particle number
Fig. 2. The error bars in the figure represent standard concentrations from log burning in different combustion
deviations in four repeated burnings. systems which varied from 0.4  104 to 1.5  107 parti-
For all of the gaseous pollutants measured in our study, cles cm3 (Wieser and Gaegauf, 2005). The particle number
the emission factors of CO and CO2 followed the order of emission factors were (1.8  0.1)  1013, (1.0  0.1)  1013,
wheat straw > corn straw > rice straw, while the NOx EFs and (1.7  0.1)  1013 particles kg1 for rice, wheat, and
were in the order of rice straw > corn straw > wheat straw. corn straws, respectively. It may be seen that particle
The differences in EFs were attributed to the fact that the number emission factors from the burning of rice and corn
wheat and corn straws used in this experiment were straws were higher than those from wheat straw. Due to
planted in northern China while the rice straw was from the absence of data on particle number emission factors for
southeastern China. Different growing regions could be crop residue burning, we compared our results with those
responsible for the different C, N contents in wheat, corn

Table 1
Emission factors of gas pollutions emitted from burning of rice, wheat and corn straws (g kg1)a

Chemical species Rice straw (n ¼ 4) Wheat straw (n ¼ 4) Corn straw (n ¼ 4) Literature


CO 64.2  4.9 141.2  14.8 114.7  12.4 52.9  8.0,b 92  84,d 99.9  32.7,g 60  23,i 53  4.0i
CO2 791.3  12.5 1557.9  85.8 1261.5  59.9 1515  177,d 1787  36,e 1400,f 1225  101,g 1540–1615,h
1470  46,i 1350  16i
NO2 0.79  0.05 0.32  0.06 0.43  0.03 0.56  0.47e
NO 1.02  0.03 0.79  0.13 0.85  0.06 0.78  0.71e
NOx 1.81  0.09 1.12  0.19 1.28  0.04 2.63,c 2.5  1.0,d 1.70  1.68,e 3,f 0.89  0.48,g 3.3  1.7,i 4.3  1.8i
a
Dry fuel mass basis. The result in our study was given as average emission factor and standard deviation.
b
Dhammapala et al. (2006); wheat.
c
Dennis et al. (2002); wheat.
d
Andreae and Merlet (2001); agricultural residue.
e
Sahai et al. (2007); wheat straw.
f
de Zarate et al. (2000); cereal waste.
g
Zhang et al. (2000); wheat residue burned as fuel.
h
Air Sciences Inc (2003a,b); wheat residue.
i
Li et al. (2007); wheat straw and corn stover.
8436 H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441

Table 2
Particle number concentrations and particle number emission factors from burning of rice, wheat and corn straws

Type of crop residue Rice straw Wheat straw Corn straw


Parameter Chamber temp. ( C)a 24.1 27.5 23.7
Chamber RH (%)b 71.3 58.9 69.3
Num.c 4 4 4

Particle number Maxd (particles cm3) 7.9  104 4.9  104 8.7  104
concentration Mine (particles cm3) 6.7  104 3.2  104 6.9  104
Mean (particles cm3) 7.3  104 3.9  104 7.5  104
SDf 0.3  104 0.7  104 0.6  104
CVg 0.05 0.17 0.08

Particle number emission factor (particles kg1) (1.8  0.1) 1013 (1.0  0.1) 1013 (1.7  0.1)1013
a
Average temperature.
b
Average relative humidity.
c
Number of experiments.
d
Maximum.
e
Minimum.
f
Standard deviation.
g
Coefficient of variance (CV ¼ SD/mean).

reported by Wardoyo et al. (2006), who presented them for The NOx ER was comparable with the data from Andreae
slow burning conditions. The average particle number (1991) and Lacaux et al. (1996). However, our result was
emission factors in their work were in the range of 2.8– higher than those of Crutzen and Andreae (1990) and
44.8  1013 particles kg1 for woods, 0.5–9.3  1013 parti- Delmas et al. (1995), which could probably be explained by
cles kg1 for leaves and branches, respectively. Our results the fact that NOx emissions are related to the nitrogen
were consistent with these previous studies. content of the biofuel (Prasad et al., 2000; Lee et al., 2005).
It is well known that flaming and smoldering combus-
3.2. Emission ratio of CO and NOx and modified combustion tion is less separated during the measurements of real-
efficiency (MCE) world fires. Each fuel corresponds to a multicycle burn of
ignition, flaming, and smoldering stages. Combustion
Emission ratio (ERs) of CO and NOx to CO2 from rice, phases of real-world fires can be divided using combustion
wheat and corn straw burning are shown in Table 3, in efficiency (CE). Alternatively, if only CO2 and CO are
which the mean values were derived from the averaging of measured, the modified combustion efficiency (MCE) can
four burnings for each fuel type. be used to distinguish flaming and smoldering combustion
In our study, the emission ratios (ERs) of CO to CO2 were ðMCE ¼ C½CO2  =ðC½CO2  þ C½CO ÞÞ. The flaming combustion
8.1  0.7% for rice straw, 9.1  0.5% for wheat straw, and usually exhibits the highest MCE (0.9–1) (Reid et al., 2005),
9.1  0.7% for corn straw, respectively. Crutzen and Andreae suggesting the remarkable influence of modified combus-
(1990) reported that the typical ER of CO to CO2 was lower tion efficiency (MCE) on the partition of flaming and
than 0.1 during the flaming phase, while during the smol- smoldering. Modified combustion efficiency (MCE) in our
dering phase it could increase up to 0.2–0.3. It may clearly study was 0.93, 0.92, and 0.92 for rice, wheat, and corn
be seen that the ER of CO to CO2 in our experiment was straw, respectively (Table 3). This suggested that the
much less than 0.1, indicating that the burning of crop burning process of agricultural crop residue was dominated
residue was dominated by the flaming phase. Moreover, by the flaming combustion in our laboratory tests.
the ER of CO to CO2 in our tests was found to be similar to
those determined from other biofuels and burning prac- 3.3. Yield estimate of agricultural crop residue
tices in the literature (Hurst et al., 1994; Lacaux et al., 1996;
Ward and Hardy, 1991; Cofer et al., 1991). ER of NOx to CO2 In order to evaluate emissions of gaseous pollutants from
averaged at 0.19  0.03% for rice straw, 0.07  0.005% for the burning of rice, wheat and corn straws – the three major
wheat straw, and 0.10  0.005% for corn straw, respectively. agricultural residues in China, we first need to estimate the

Table 3
Emission ratio (ER) and modified combustion efficiency (MCE) from burning of rice, wheat and corn straws

Rice straw Wheat straw Corn straw

CO/CO2 NOx/CO2 MCE CO/CO2 NOx/CO2 MCE CO/CO2 NOx/CO2 MCE


1 0.092 0.0014 0.915 0.096 0.0006 0.912 0.076 0.0010 0.929
2 0.083 0.0019 0.924 0.081 0.0007 0.925 0.095 0.0009 0.913
3 0.068 0.0025 0.936 0.090 0.0008 0.918 0.098 0.0011 0.911
4 0.082 0.0019 0.924 0.096 0.0007 0.913 0.093 0.0010 0.915
Ava 0.081 0.0019 0.925 0.091 0.0007 0.917 0.091 0.0010 0.917
SDb 0.007 0.00030 0.006 0.005 0.00005 0.005 0.007 0.00005 0.006
a
Average value.
b
Standard deviation.
H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441 8437

Table 4
National and provincial estimated amounts of agricultural crop residue (rice, wheat and corn straws) and those burned in the field and as domestic fuel in
2004 (Gg)

Province Agricultural crop residue (Gg) Agricultural crop residue burned in the Agricultural crop residue burned as
field (Gg) domestic fuel (Gg)

Rice straw Wheat straw Corn straw Rice straw Wheat straw Corn straw Rice straw Wheat straw Corn straw
Beijing 6.29 251.48 644.00 2.83 113.17 289.80 1.60 51.05 159.07
Tianjin 35.20 490.53 1296.20 14.26 198.66 524.96 8.98 99.58 320.16
Hebei 255.80 13,917.22 21,471.40 61.90 3367.97 5196.08 28.91 1572.65 2426.27
Shanxi 7.73 3496.69 9539.00 1.61 730.81 1993.65 0.46 206.30 562.80
Neimenggu 280.35 1078.59 17,774.00 59.71 229.74 3785.86 71.49 218.95 4390.18
Liaoning 2189.22 84.69 18,144.00 461.93 17.87 3828.38 757.47 29.30 6277.82
Jilin 1982.39 81.96 32,306.00 414.32 17.13 6751.95 505.51 16.64 7979.58
Heilongjiang 5250.64 542.30 16,618.00 1176.14 121.48 3722.43 1160.39 119.85 3672.58
Shanghai 512.11 100.95 63.00 249.40 49.16 30.68 152.61 30.08 18.77
Jiangsu 8750.91 8314.98 3945.00 2992.81 2843.72 1349.19 2966.56 2818.78 1337.36
Zhejiang 4030.19 284.67 430.00 1716.86 121.27 183.18 673.04 47.54 71.81
Anhui 6003.85 8780.65 5212.00 1122.72 1641.98 974.64 1050.67 1536.61 912.10
Fujian 3261.03 37.84 232.40 1059.84 12.30 75.53 136.96 1.59 9.76
Jiangxi 8476.16 39.48 125.40 1839.33 8.57 27.21 1000.19 4.66 14.80
Shandong 485.25 21,378.31 28,220.40 128.59 5665.25 7478.41 95.11 4190.15 5531.20
Henan 1496.26 31,315.55 15,326.20 294.76 6169.16 3019.26 335.16 7014.68 3433.07
Hubei 8356.24 2259.64 3350.00 1955.36 528.76 783.90 3877.29 1048.47 1554.40
Hunan 12,897.22 225.25 2571.00 2876.08 50.23 573.33 877.01 15.32 174.83
Guangdong 7292.22 22.27 1062.60 2654.37 8.10 386.79 1531.37 4.68 223.15
Guangxi 7492.82 23.77 3194.00 1251.30 3.97 533.40 1910.67 4.82 788.92
Hainan 893.38 0.00 122.80 269.80 0.00 37.09 89.34 0.00 12.28
Chongqing 3097.18 1144.71 4140.00 600.85 222.07 803.16 789.78 232.38 1022.58
Sichuan 9170.00 5821.89 10,346.00 1824.83 1158.56 2058.85 4915.12 3120.53 5545.46
Guizhou 2861.44 1019.04 6398.00 429.22 152.86 959.70 572.29 203.81 1279.60
Yunnan 3961.59 1698.62 7998.60 451.62 193.64 911.84 1010.21 344.82 1975.65
Xizang 3.49 371.96 32.40 0.30 31.62 2.75 0.89 75.51 8.00
Shananxi 470.37 5402.53 7464.00 69.61 799.57 1104.67 119.47 1372.24 1895.86
Gansu 22.30 3721.80 4888.60 3.70 617.82 811.51 4.55 759.25 997.27
Qinghai 0.00 502.69 0.00 0.00 50.77 0.00 0.00 102.05 0.00
Ningxia 230.76 1032.83 2398.60 46.38 207.60 482.12 63.69 285.06 662.01
Xinjiang 316.05 4700.41 6346.80 60.68 902.48 1218.59 80.59 954.18 1567.66

Total 100,088.44 118,143.29 231,660.40 24,091.12 26,236.29 49,898.92 24,787.37 26,481.53 54,824.99

Bold indicated that the burning ratio of agricultural crop residue burned as domestic fuel was referred to the national average level.

amount of agricultural crop residue. Based on extensive to estimate the proportion of crop residue burned openly
survey data, Gao et al. (2002) presented the percentage in the field.
of crop residue used as domestic fuel in 21 provinces of National and provincial estimates of the amounts of
China. Compared with the corresponding government- agricultural crop residue and those burned as domestic fuel
generated statistics, the percentage of crop residue burned and in the field in China for 2004 are shown in Table 4. Data
for domestic fuel in individual provinces seems more are derived from 31 provinces. The total amounts of agri-
reasonable and agrees better with other survey results (Yan cultural crop residue in China for the year 2004 were
et al., 2006). So we used Gao et al.’s percentage data to 100.09, 114.18, and 231.66 Tg for rice, wheat, and corn
estimate the amount of crop residue burned as domestic fuel straws, respectively, and the estimates for the amounts
for the year 2004. For provinces not listed by Gao et al. burned as domestic fuel were 24.09, 26.24, and 49.89 Tg for
(2002), the average percentages for crop residue burned for rice, wheat, and corn straws, respectively, while the
fuel for the whole country were adopted, i.e. 25.5%, 20.3%, amounts consumed by open burning were 24.79, 26.48,
and 24.7% for rice, wheat, and corn straws, respectively. and 54.82 Tg for rice, wheat, and corn straws, respectively.
Agricultural crop residues are not only burned as We estimated that w106 Tg agricultural crop residue
domestic fuel, they are also burned directly in the field, was burned as domestic fuel in 2004, which was w23.6%
especially during harvest seasons, which can result in of total crop residue production. Our estimate was lower
serious local and regional environmental pollution (Guo than the result of Yan et al. (2006), who reported that
et al., 2004; Duan et al., 2004). Although the open burning w153 Tg crop residue was burned as domestic fuel in 2000
of crop residue has been a common practice in China, (about 24.4% of the total crop residue). This suggested that
unfortunately, the literature related to open burning of the crop residue burned as domestic fuel was decreasing
agricultural waste is limited (Li et al., 2007). Cao et al. gradually due to the increase in other energy use. We also
(2006) deduced that the amount of crop residue openly evaluated that w100 Tg crop residue in 2004 was openly
burned was proportional to peasants’ income level, and burned, which was w22.3% of the total crop residue.
this hypothesis was supported by investigations in Henan Compared with the data derived from Yan et al. (2006)
Province (Chen, 2001). Consequently, we used this method (w122 Tg in 2000 was burned in the field, accounting for
8438 H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441

Table 5
Total emissions of gaseous pollutants from agricultural crop residue (rice, wheat and corn straws) burned as domestic fuel and in the field

Province Total emissions from agricultural crop residue burned as domestic fuel and in the field (rice, wheat and corn straws)

CO (Gg) CO2 (Gg) NO2 (Gg) NO (Gg) NOx (Gg)


Beijing 74.96  8.02 825.59  41.02 0.25  23.54 0.52  0.05 0.77  0.05
Tianjin 140.54  15.01 1549.14  76.05 0.48  0.04 0.98  0.09 1.46  0.09
Hebei 1577.73  168.08 17,384.43  881.62 4.93  0.53 10.47  1.10 15.45  1.25
Shanxi 425.68  45.58 4686.53  233.56 1.40  0.13 2.92  0.28 4.33  0.28
Neimenggu 1009.57  108.67 11,116.92  529.88 3.76  0.28 7.44  0.55 11.21  0.42
Liaoning 1244.13  131.99 13,787.38  624.65 5.32  0.37 9.87  0.65 15.19  0.52
Jilin 1753.53  187.67 19,364.30  896.41 7.07  0.49 13.49  0.92 20.56  0.68
Heilongjiang 1032.29  106.72 11,553.67  492.87 5.10  0.35 8.86  0.55 13.97  0.55
Shanghai 42.67  3.76 503.95  14.78 0.36  0.03 0.51  0.03 0.88  0.05
Jiangsu 1490.28  146.32 16,926.33  721.26 7.67  0.72 12.84  1.08 20.57  1.72
Zhejiang 206.52  17.37 2475.79  59.63 2.05  0.14 2.79  0.11 4.84  0.26
Anhui 804.76  81.09 9051.87  412.91 3.54  0.36 6.33  0.59 9.91  0.88
Fujian 88.58  7.13 1076.26  21.26 0.98  0.06 1.30  0.04 2.29  0.11
Jiangxi 188.98  14.63 2320.51  39.14 2.27  0.14 2.94  0.09 5.21  0.26
Shandong 2898.15  308.28 31,942.36  1627.67 8.92  0.99 19.07  2.07 28.09  2.41
Henan 2642.08  278.22 29,177.19  1525.54 7.49  1.02 16.54  2.12 24.17  2.82
Hubei 865.36  80.92 10,022.31  348.29 6.12  0.46 9.18  0.52 15.32  0.92
Hunan 336.02  28.64 4015.75  97.35 3.31  0.21 4.52  0.17 7.82  0.38
Guangdong 340.49  28.26 4101.51  89.95 3.57  0.23 4.79  0.16 8.37  0.40
Guangxi 355.91  32.02 4183.87  119.48 3.07  0.19 4.36  0.18 7.43  0.34
Hainan 28.72  2.37 346.46  7.44 0.30  0.02 0.41  0.01 0.71  0.03
Chongqing 362.86  36.18 4111.57  165.74 2.03  0.15 3.33  0.21 5.36  0.28
Sichuan 1909.13  190.65 21,592.55  906.89 9.96  0.82 16.72  1.21 26.73  1.72
Guizhou 371.51  37.95 4173.01  177.25 1.87  0.14 3.21  0.21 5.08  0.25
Yunnan 501.08  50.94 5638.19  237.43 2.57  0.19 4.37  0.29 6.94  0.35
Xizang 16.44  1.72 181.39  9.85 0.04  0.01 0.09  0.01 0.14  0.02
Shananxi 662.96  70.28 7318.26  368.44 2.13  0.23 4.46  0.47 6.62  0.55
Gansu 402.44  42.85 4433.64  226.60 1.22  0.14 2.63  0.29 3.87  0.33
Qinghai 21.58  2.26 238.07  13.11 0.05  0.01 0.12  0.02 0.17  0.03
Ningxia 207.86  22.01 2297.94  112.17 0.74  0.07 1.47  0.14 2.22  0.15
Xinjiang 590.81  62.72 6519.13  327.96 1.90  0.20 3.98  0.41 5.90  0.48

Total 22,593.59  23,18.31 25,2915.90  11,407.13 100.52  8.75 180.52  14.60 281.56  18.60

w19.4% of the total crop residue), our estimates were pollutant emissions were caused by corn straw burning,
lower in total amounts but slightly higher in relative which accounted for approximately half of the total
amounts. emissions.

3.4. Emission inventory of gaseous pollutants 3.5. Emission allocation of gaseous pollutants

National and provincial emissions of gaseous pollutants A simple GIS was applied to display emission allocation
(CO, CO2, NO, NO2 and NOx) from agricultural crop residue of gaseous pollutants from the burning of agricultural crop
burning in China for 2004 are compiled in Table 5. residue. Emission conditions of gaseous pollutants for the
Total emissions of gaseous pollutants were estimated year 2004 at province-level in China are shown in Fig. 3.
to be 22.59  2.32 Tg CO, 252.92  11.41 Tg CO2, and Different emission regions can be distinguished by
281.56  18.60 Gg NOx, respectively. The top five contributors different emission strengths per km2. The highest CO, CO2
by province are Shandong, Henan, Sichuan, Jilin, and Jiangsu, and NOx emission fluxes were from Shandong, Henan and
which were also the regions with high income levels of Jiangsu provinces, where the rural population density and
peasants and rural population densities. economic levels were relatively higher than in other
Calculated gaseous pollutant emissions from rice, provinces. The lowest CO, CO2 and NOx gaseous pollutant
wheat, and corn straws burned as domestic fuel and in the releases were in Inner Mongolia and the western part of
field are presented (see Supplementary Information SI China, which were coincided with lower rural population
Tables 1–3). Total emissions of CO, CO2, and NOx were densities and lower economic levels.
3137.99  239.50, 38,677.55  610.98, and 88.47  4.39 Gg The relative proportion of gaseous pollutant emissions
for rice straw, 7443.76  780.22, 82,129.09  4523.19, and from the burning of rice, wheat and corn straws for the year
59.04  10.01 Gg for wheat straw, and 12,011.83  1298.58, 2004 at province-level in China is shown in Fig. 4. The
13,2109.20  6272.96, and 134.05  4.19 Gg for corn straw, distribution of straw species in China is remarkable,
respectively. The percentages of CO, CO2, and NOx to the because the different straw types cause different magni-
total emissions were 13.9%, 15.3%, and 31.4% for rice straw, tudes of emission. For example, the rice straw regions are
32.9%, 32.5%, and 20.9% for wheat straw, and 53.2%, 52.2%, mainly distributed in southern China, corn straw regions in
and 47.6% for corn straw, respectively. A majority of gaseous northern and mid-China, wheat straw regions in western
H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441 8439

Fig. 3. Distributions of gaseous pollutant emissions for the year 2004 at


province-level in China: (a) CO2, (b) CO, (c) NOx. (units: kg km2).

and mid-China, respectively. In southern China, the great


Fig. 4. Relative proportion of gaseous pollutant emissions from burning of
mass of gaseous pollutant emissions came mostly from rice rice, wheat, and corn straws for the year 2004 at province-level in China: (a)
straw burning. The highest emission strength in northern CO2, (b) CO, (c) NOx.
China was caused by corn straw burning. The western part
of China was characterized by relatively high emission a burning stove and aerosol chamber. The average emission
fluxes from the burning of wheat straw. factors of CO2, CO, NO, NO2, and NOx were 791.3, 64.2, 1.02,
0.79, and 1.81 g kg1 for rice straw, 1557.9, 141.2, 0.79, 0.32,
4. Conclusions and 1.12 g kg1 for wheat straw, and 1261.5, 114.7, 0.85,
0.43, and 1.28 g kg1 for corn straw, respectively. Accord-
Gaseous pollutants and particle number emitted from ingly, the mean emission factors of particle number (PN)
agricultural crop residue burning were investigated using were 1.8  1013, 1.0  1013, and 1.7  1013 particles kg1 for
8440 H. Zhang et al. / Atmospheric Environment 42 (2008) 8432–8441

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