Emission Characteristics of Particulate Matter from Rural

Household Biofuel Combustion in China

Xinghua Li, Lei Duan, Shuxiao Wang, Jingchun Duan, Xingming Guo, Honghong Yi,
Jingnan Hu, Chao Li, and Jiming Hao*
Department of EnVironmental Science and Engineering, Tsinghua UniVersity, Beijing 100084, China
ReceiVed April 6, 2006. ReVised Manuscript ReceiVed October 9, 2006
Field measurements in rural households were conducted in three Chinese municipalities/provinces (Beijing,
Chongqing, and Henan) to determine the emission characteristics of particulate matter from biofuel combustion.
The selected biofuel types and stove types are representative of local rural areas. Particle number concentration,
size distribution, and mass size distribution were determined. Both the particle number and mass of these
emissions were dominated by submicrometer particles. The emission factor of PM2.5 from combustion is
between 1.80 and 7.00 g/kg of biofuel (dry basis) and 0.84-2.40 g/MJ of delivered energy and is averaged to
4.21 g/kg of biofuel (dry basis) and 1.46 g/MJ delivered energy. In this study, it appears that particle emissions
can be correlated with combustion conditions and stove configuration. Particle emissions are the highest during
the high power phase. Unfortunately, the more thermally efficient stove has higher per kilogram fuel particulate
matter (PM) emissions than the less thermally efficient stoves, that is, the increase in thermal efficiency cannot
offset the increase in particle emissions.
Introduction
With the rapid development of the economy and society,
commercial energy, such as electricity and liquid propane gas
(LPG), is becoming more popular in Chinas rural households.
However, biofuel, such as crop waste and wood, still dominates
the rural energy supply in China. In 2000, 288 million tons of
agricultural biomass and 141 million tons of firewood were
directly burned by rural households for cooking and heating,
contributing 57% of total rural household energy use (353
million tons of coal equivalent).
1,2
Patterns of energy use in
Chinas rural households, which are dominated by biofuels, will
not change significantly for a long time. Unfortunately, biofuel
combustion is mainly carried out in small household stoves
under poor combustion conditions and without any emission
control. This results in high levels of particulate matter, CO,
polycyclic aromatic hydrocarbons (PAHs), and other air pol-
lutant emissions, which cause high levels of indoor air pollution,
3
local air pollution,
4
and regional and global climate impacts.
5,6
The particulate matter contains a large carbonaceous fraction,
i.e., organic carbon (OC) and black carbon (BC). BC is thought
to absorb solar radiation and contribute to global warming.
6
Street et al. estimated that BC emissions from biofuel combus-
tion in China were 512 Gg in 1995, comprising 38% of the
total national emissions.
7
OC contains a multitude of organic
compounds, some of which are carcinogenic and mutagenic,
such as polycyclic aromatic hydrocarbons (PAHs).
8,9
In view of the adverse effect of particulate matter emitted
from biofuel combustion, it is necessary to know the emission
characteristics so as to reduce the emissions. A few studies on
emissions from household stoves in developing countries have
been conducted. For these small combustion devices, three major
types of methods are used to determine emissions: the chamber
method, hood method, and the carbon balance approach.
10
Joshi
et al. adopted the chamber method to study CO and total
suspended particle (TSP) emissions from burning biofuels in
metal cook stoves and found that the more efficient stoves have
higher emission factors of both CO and TSP for all three biofuels
tested.
11
Ballard-Tremeer et al. used the hood method to compare
efficiencies and emissions of five rural, wood-burning cooking
devices and observed that the average emissions of TSP were
lowest for the improved open fire and the two-pot ceramic
stove.
12
Venkataraman et al. adopted the hood method and a
dilution sampler to measure CO, size-resolved aerosols, and
PAH emissions from biofuel combustion in India.
13,14
However,
studies of the emission characteristics of particulate matter from
* Author to whom correspondence should be addressed. Telephone:
+86-10-62782195. Fax: +86-10-62773650. E-mail address:
hjm-den@tsinghua.edu.cn.
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Bo, Y. Atmos. EnViron. 2001, 35, 4281-4296.
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1992, 26, 1278-1284.
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Lafleur, A. L.; Cass, G. R. EnViron. Sci. Technol. 2005, 39, 9547-9560.
(10) Mitra, A. P.; Morawska, L.; Sharma, C.; Zhang, J. Chemosphere
2002, 49, 903-922.
(11) Joshi, V.; Venkataraman, C.; Ahuja, D. R. EnViron. Manage. 1989,
13, 763-772.
(12) Ballard-Tremeer, G.; Jawurek, H. Biomass Bioenerg. 1996, 11, 419-
430.
(13) Venkataraman, C.; Rao, G. U. M. EnViron. Sci. Technol. 2001, 35,
2100-2107.
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Sci. 2003, 33, 503-518.
845 Energy & Fuels 2007, 21, 845-851
10.1021/ef060150g CCC: $37.00 2007 American Chemical Society
Published on Web 03/07/2007
rural household biofuel combustion in China are limited. Smith
et al. studied greenhouse gas and other airborne pollutions
(including TSP) emissions from household stoves in China and
other developing countries using the carbon balance approach.
15-17
The purpose of this paper is to provide an initial assessment of
particulate matter emissions from typical rural household
biofuels and stove combinations used in China. Therefore, the
objectives of this study were to (a) measure particle number
concentration, size distribution, and mass size distribution; (b)
quantify PM2.5 emission factors, and (c) relate these to stove
configuration, fuel, and combustion conditions.
Methods
Selection of Biofuels and Stoves to Test. In Chinas rural
households, crop waste which is used as fuel to burn in the
household stoves for cooking and heating include the following:
rice straw, wheat residue, maize residue, bean straw, cotton stalk
and kaoliang stalk, and so on. Fuel wood and branches are also
often used as rural household fuel. Improved stoves have become
popular in rural households. These are stoves with an enclosed
combustion chamber and a flue. About 190 million improved stoves
have been installed, accounting for 80% of rural households.
1
In
the northern rural areas, stove/kang is used commonly for cooking
and heating. Kang is a bed made of brick or clay, with passageways
inside it, and flue gas, after leaving the stove, passes through the
passageways and transfers heat to the kang.
Three Chinese municipalities/provinces (Beijing, Chongqing, and
Henan), located in the north, southwest, and the middle of China,
respectively, were chosen for field measurement. Tests were carried
out in local rural households. Before determining the fuel/stove
combination to be tested, investigations were carried out. The
selected fuels and stove types are representative of the local rural
area. In Chongqing, an improved stove and five typical biofuel
types, rice straw, maize residue, bean straw, fuel wood, and
branches, were selected for this study. The stove has two combus-
tion chambers, two fuel inlets, two main pots, one auxiliary pot,
and a flue. One combustion chamber burns biofuel, and the other
burns coal. The former has no bottom grate. Fuel is burned in the
combustion chambers, and heat is transferred to the main pot while
the flue gas is drawn through the duct to the flue. The auxiliary
pot is located in the duct and uses the remaining heat energy of
flue gas. Fuel could be burned in both combustion chambers
simultaneously or only in one chamber. When one chamber is used,
the duct of the other chamber connecting it to the flue is closed.
This study is conducted only with the combustion chamber that
burns biofuel. In Henan, three different biofuels typical of the area,
wheat residue, kaoliang stalk, and cotton stalk, were chosen to burn
in a local typical improved stove. The stove has almost the same
configuration as stoves in Chongqing. Both combustion chambers
burn biofuel and have a bottom grate. The experiment was carried
out in one combustion chamber. In Beijing, branches and a stove/
kang were selected as the fuel/stove combination. The stove has
one combustion chamber, one fuel inlet, and one main pot.
All the selected stoves were made of brick, and their configu-
ration parameters are shown in Table 1. The proximate and ultimate
analyses of the tested fuels are listed in Table 2. According to local
cooking habits, the tested crop wastes were wrapped into batches
of 20-25 cm in length and woody fuel was cut into pieces about
20 cm long.
Definition of the Burning Cycle. Cooking is not a steady
process causing emissions from the biofuel combustion to vary
during the cooking.
16
Therefore, it is necessary to choose a burning
cycle similar to the common cooking practice in the field. The most
common cooking practices include high power and low power
phases. High power phase means heating a quantitative amount of
water from the ambient water temperature to the boiling temperature
as rapidly as possible. A low power phase would involve the water
simmering at the lowest power. The water-boiling test
18
was
adopted with slight modification according to a Chinese standard
method
19
to define a burning cycle. The water-boiling test is
described as follows:
(15) Zhang, J.; Smith, K. R.; Ma, Y.; Ye, S.; Jiang, F.; Qi, W.; Liu, P.;
Khalil, M. A. K.; Rasmussen, R. A.; Thorneloe, S. A. Atmos. EnViron.
2000, 34, 4537-4549.
(16) Smith, K. R.; Khalil, M. A. K.; Rasmussen, R. A.; Thorneloe, S.
A.; Manegdeg, F.; Apte, M. Chemosphere 1993, 26, 479-505.
(17) Smith, K. R.; Uma, R.; Kishore, V. V. N.; Lata, K.; Joshi, V.; Zhang,
J.; Rasmussen, R. A.; Khalil, M. A. K. Greenhouse gases from small-scale
combustion deVices in deVeloping countries, phase IIa: household stoVes
in India; Office of Research and Development, US EPA: Washington, DC,
1999.
(18) VITA (Volunteers in Technical Assistance, Inc.). Testing the
efficiency of wood-burning cookstoVes; International Standards: Arlington,
VA, 1985.
(19) Standardization Administration of the Peoples Republic of China
(SAC). Testing method for the heat characteristics of firewood stoVes;
SAC: Beijing, China, 1984.
Table 1. Stove Configuration Parameters
location description
combust
chamber
volume (m
3
)
grate to
pot-bottom
distance (m)
grate
air-inlet
area (m
2
)
fuel
inlet
area (m
2
) fuel used
Chongqing improved stove, one main pot
and one auxiliary pot, no grate
0.060 0.23 no grate 0.045 rice straw, maize residue,
bean straw, fuel wood branch
Henan improved stove, one main pot and
one auxiliary pot, bottom grate
0.034 0.13 0.016 0.041 wheat residue, kaoliang stalk,
cotton stalk
Beijing stove/kang, one pot, no grate 0.039 0.20 no grate 0.042 branch
Table 2. Tested Fuels Proximate and Ultimate Analysis
fuel
rice
straw
maize
residue
bean
straw
fuel
wood branch (I)
cotton
stalk
wheat
residue
kaoliang
stalk branch (II)
Proximate (as Received, mass %)
moisture 6.24 6.49 10.07 7.51 7.90 8.40 5.42 5.47 7.06
volatile matter 62.50 70.33 71.35 76.14 73.16 70.83 68.74 72.27 75.33
fixed carbon 16.56 16.87 15.59 14.41 17.14 17.54 18.07 17.98 16.71
ash 14.70 6.31 2.99 1.94 1.80 3.23 7.77 4.28 0.90
Ultimate (Dry Basis, mass %)
C 41.42 46.32 47.54 50.68 48.96 49.50 44.64 47.76 49.90
H 5.57 6.09 6.35 6.37 6.23 6.28 5.85 6.12 6.36
N 0.94 1.62 1.15 0.29 0.76 1.25 0.56 0.59 0.70
S 0.16 0.15 0.16 0.018 0.053 0.010 0.20 0.078 0.037
O (by difference) 39.43 39.07 41.48 40.54 42.05 39.43 40.53 40.92 42.03
low heating value
(dry basis, MJ/kg)
15.67 17.54 17.86 19.11 18.21 18.71 16.61 17.89 18.69
846 Energy & Fuels, Vol. 21, No. 2, 2007 Li et al.
Fill the stove pot (including the main and auxiliary pots) to
2
/
3
of its capacity with room temperature water.
Weigh out a quantity of biofuel such that its weight is about
1
/
3
-
1
/
2
of the water weight in the main pot.
Cover the pot with a lid and a thermometer is inserted through
the lid into the water.
Start the fire at high power to bring the water in the main pot
to boil.
Continue the test at low power using the remaining biofuel.
Terminate the test when the water temperature in the main pot
dropped by about 1 C.
Bail out the water in the pot and weigh it.
Extinguish the ash and any unburned fuel residue by shutting
off access to air, and weigh them after they are cool.
Prior to the planned sampling for each fuel/stove combination,
trial tests were performed to standardize the burning cycle.
Preliminary tests were carried out until a satisfactory method
precision (relative standard deviation less than 20%) for the main
parameters, i.e., time to boil, time of burning cycle, and thermal
efficiency, was obtained. The time for completion of the burning
cycle ranged from 30-50 min for most of the test.
During the whole burning cycle, biofuels were manually fed into
the stove in batches. The time, temperature, and weight of water
were recorded at the beginning and end of the burning cycle, and
the amount of biofuel burned was also recorded. Stove thermal
efficiency can be determined according to these data. The sampling
period covered the whole burning cycle from the moment of the
beginning of the burn (biofuel had been ignited) to the end of the
burning process (the water temperature in the main pot dropped
by about 1 C).
Sampling Approach. An outline of the sampling system is
shown in Figure 1. It includes a dilution sampling system, particle
measurement, and flue gas monitoring. The system is described in
more detail in the following subsection.
Dilution Sampling System. The dilution sampling system simu-
lates the cooling and dilution processes after the hot flue gas leaves
the stack and is widely used for characterizing emissions from
stationary combustion sources.
20
A compact dilution sampling
system was developed for this field study that consists of four main
parts: sampling inlet, dilution part, residence chamber, and sampler.
In the sampling inlet part, flue gas is withdrawn from the flue,
put through a cyclone separator, and then advanced to the first
dilution. The cyclone, which removes particles larger than 10 m,
is installed outside the flue because the flue is not large enough to
accommodate it. The sampling inlet was heated to about 150 C to
reduce particle thermophoresis losses. Because the flue gas velocity
in the flue is unstable, isokinetic sampling cannot be achieved. The
sampling error arising from the velocity mismatch can be neglected
for particles with diameters less than 2.5 m.
21
The dilution part consists of two stage diluters. The operation
principle of the first diluter is based on an ejection type dilution
(Dekati Ltd, Finland). The ejector diluter is used to keep the dilution
ratio constant at about 10. About 0-50 L/min can be drawn from
the outlet of the diluter to the second diluter according to research
requirements. The second diluter is a cylindrical enclosure with a
perforated plate inside. The sample flow from the first diluter is
introduced inside the enclosure, and the dilution air is forced through
the apertures of the plate into the enclosure where it mixes with
the sample flow. Two vortex flow meters record sample flow from
the first diluter and the dilution air flow rate in the second diluter.
The second diluter can supply a dilution ratio from 1 to 10. The
total range of the dilution ratio is from 10 to 100. An oil-free air
compressor and a pump supply the first and second diluters dilution
air, respectively; the air must be purified before entering into the
dilutor.
All of the diluted sampling gas is transferred to the residence
chamber. The temperature, relative humidity, and pressure in the
chamber are monitored.
The sampler is attached to the end of the residence chamber and
has eight sampling ports for connecting with particle measurement
instruments. In this study, an electrical low-pressure impactor,
(ELPI, Dekati Ltd., Finland)
22
and three parallel PM2.5 cyclones
with filter packs were used to collect particles. The gas in the
chamber is under a small positive pressure, and extra gas can be
automatically discharged from the unused sampling ports. The
whole dilution sampling system has shown considerable stability.
The sampler is made entirely from stainless steel, copper, and
Teflon. A dilution air ratio of about 20 and an aging time of about
80 s were applied in the study.
Particle Measurement. ELPI was used to measure in the real-
time particle number concentration and size distribution. Operating
at a flow rate of 9.89 L/min, the ELPI has 50% cut-point
aerodynamic diameters of 0.028, 0.056, 0.095, 0.157, 0.263, 0.382,
0.613, 0.948, 1.600, 2.390, 4.000, 6.680, and 9.920 m on stages
1-13. Our focus was on the lower ELPI stages 1-9 which
characterized the particle size distribution range of 0.028-2.390
m, the typical particle distribution range of biofuel combus-
tion.
13,23-25
Greased and baked aluminum foils of 25 mm in diameter
were used as collection foils.
A low pressure impactor (LPIswhen ELPI is used without the
electrical charger) was used to determine particle mass size
distribution over the range of 0.028-2.390 m. In the upper four
stages, aluminum foils were coated with high vacuum grease to
prevent particle bounce. For further size resolved chemical analysis,
the lower nine stages were not greased to avoid interference. Particle
bounce within the lower impactor stages was not a problem.
24
(20) Hidemann, L. M.; Cass, G. R.; Markowski, G. R. Aerosol Sci. Tech.
1989, 10, 193-204.
(21) Hinds, W.C. Aerosol technology: properties, behaVior, and mea-
surement of airborne particles; John Wiley & Sons, Inc.: New York, 1999.
(22) Keskinen, J.; Pietarinen, K.; Lehtimaki, M. J. Aerosol Sci. 1992,
23, 353-360.
(23) Purvis, C. R.; McCrillis, R. C.; Kariher, P. H. EnViron. Sci. Technol.
2000, 34, 1653-1658.
(24) Kleeman, M. J.; Schauer, J. J.; Cass, G. R. EnViron. Sci. Technol.
1999, 33, 3516-3523.
(25) Hays, M. D.; Smith, N. D.; Kinsey, J.; Dong, Y.; Kariher, P. J.
Aerosol Sci. 2003, 34, 1061-1084.
Figure 1. Outline of the sampling system.
Emission Characteristics Household Biofuel Energy & Fuels, Vol. 21, No. 2, 2007 847
Before and after sample collection, all substrates were conditioned
for 24 h at about 40% RH and 25 C in an air-conditioned room
and weighed on a microbalance with a resolution 1 g.
All number and mass concentrations measured by ELPI and LPI
were back-calculated out to the dilution air ratio at each measure-
ment and normalized to 3% CO
2
dry gas at normal temperature (0
C) and pressure (101.3 kPa).
PM2.5 was also collected by three parallel PM2.5 cyclones with
filter packs operated at 16.7 L/min. The first filter pack consisted
of a 47 mm Teflon-membrane filter for mass by gravimetric and
elemental analysis. The other two filter packs consisted of a 47
mm quartz-fiber filter for carbon, ions, and speciated organic
compound analysis. The Teflon-membrane filters were conditioned
for 24 h at about 40% RH and 25 C in an air-conditioned room
and weighed on a microbalance with a resolution 10 g. The
chemical speciation results will be presented in a companion paper.
Flue Gas Monitoring. The concentrations of gaseous air pollut-
ants (including CO
2
, CO, SO
2
, O
2
, and NO
x
) and temperature in
the flue were continuously monitored by a flue gas analyzer (Model
KM9106, Keison). The data were recorded every 10 s by a data
logger and transmitted to a notebook PC. The instrument was
calibrated before each field study.
Determination of Emission Factors. The carbon balance
approach was used to calculate the emission factors.
15
The carbon
balance equation for combustion is based on the total carbon mass
burned being equal to the total mass of carbon emitted by both as
particles and gases. The carbon content of the tested fuels, ash,
unburned fuel residue, and PM2.5 was analyzed. The average
concentrations of CO
2
and CO over the whole burning cycle in the
flue were calculated using the data monitored by the flue gas
analyzer. The amount of total hydrocarbon was not measured in
this study. Estimation based on previous study
15
shows that error
caused by neglecting total hydrocarbon is less than 5%stherefore,
the emission factors in this study are credible.
The emission factors are reported on a dry fuel mass basis (gram
per kilogram of fuel) and on an energy basis (gram per megajoule
of delivered energy). Dry fuel mass can be converted from fuel
mass burned and fuel moisture content. The emission factor based
on delivered energy can be derived from the emission factor based
on dry fuel along with the stove thermal efficiency and fuel heating
value. For the stove-burned woody fuel, the unburned fuel residue,
i.e., char, is often used later and produces pollutants. In our study,
the pollutants generated from char secondary combustion are not
calculated in determining the emission factors.
In this paper, thermal efficiency is the ratio of energy absorbed
by the water in the pots (including the main pot and the auxiliary
pot) to the energy content of the fuel consumed. For the stove-
burned woody fuel, when calculating its thermal efficiency, the
energy content of the fuel consumed was subtracted by the energy
content of char. For stove/kang, thermal efficiency just refers to
the stove; the heat delivered to the kang is not considered.
Results and Discussion
Particle Number Concentration and Size Distribution.
Particle number concentrations for all tested biofuel combustion
during the whole burning cycle, measured by the ELPI, together
with geometric mean diameters (GMDs) are summarized in
Table 3. The average particle number concentrations within the
range of 0.03-2.39 m were between 1.0 10
7
-5.0 10
7
particles/(N cm
3
) and GMDs were between 0.11 and 0.21 m.
The particle number concentration varied 1-2 orders of
magnitude in the whole burning cycle. The results of the particle
number concentration were somewhat consistent with some
previous studies. For example, Hueglin et al.
26
reported particle
number concentrations from residential wood stoves varying
from 7.8 10
6
-4.4 10
7
particles/(N cm
3
), and Johansson et
al.
27
showed particle number concentrations from domestic
heating devices varying between 1.4 10
7
-13.4 10
7
particles/(N cm
3
).
In this study, the number concentrations in the Chongqing
stove are generally less than those measured in Henan. A
possible explanation is the difference in stove configuration.
The stove in Chongqing has the largest combustion volume,
Table 3. Particle Number Concentrations and GSD during the Whole Burning Cycle
stove Chongqing Henan Beijing
fuel rice straw maize residue bean straw fuel wood branch (I) cotton stalk wheat residue kaoliang stalk branch (II)
avg number concentration
(particles/(N cm
3
))
1.2 10
7
2.9 10
7
1.6 10
7
1.3 10
7
1.9 10
7
3.3 10
7
4.6 10
7
5.0 10
7
1.0 10
7
varied range of number
concentration
(particles/(N cm
3
))
1.1 10
6
to
4.6 10
7
1.6 10
6
to
2.5 10
8
1.3 10
6
to
7.0 10
7
2.5 10
6
to
1.5 10
8
2.1 10
6
to
4.3 10
8
3.3 10
6
to
2.6 10
8
5.4 10
6
to
1.0 10
8
1.2 10
7
to
1.3 10
8
1.2 10
6
to
7.1 10
7
GMD (m) 0.11 0.14 0.17 0.15 0.12 0.13 0.16 0.11 0.21
Figure 2. Particle average number size distribution during the whole burning cycle. (Note: SC, SH, and SB denote the stoves in Chongqing,
Henan, and Beijing, respectively.)
848 Energy & Fuels, Vol. 21, No. 2, 2007 Li et al.
which can provide a relatively long time for the combustion of
volatiles released from pyrolysis of biofuel and, therefore,
decreased particle formation from incomplete combustion. The
Beijing stove/kang has the least number concentration and the
highest GMD, which may be related to its peculiar configuration.
Before being drawn to the flue, flue gas, after leaving the stove,
passes through the passageways inside the kang and transfers
heat to the kang thereby losing temperature. Flue gas residence
time in the kang is over 100 ssenough time for particle
coagulation and condensation growth that could decrease particle
number concentration and shift the GMD toward a high value.
Particle number size distributions are given in Figure 2. They
are mainly unimodal during the whole burning cycle, with a
peak between 0.12 and 0.32 m. However, they are bimodal
for branches burned in the Chongqing stove and wheat residue
and kaoliang stalk in the Henan stove, with a nucleation mode
peak less than 0.04 m and an accumulation mode peak near
0.12 m.
Particle number concentrations and size distributions during
the whole burning cycle were strongly related to the phase of
the cooking practice. Typical particle number concentrations
and size distributions during the different phases of the burning
cycle are shown in Figures 3 and 4, respectively.
In this study, the lower power phase was divided into two
parts: the earlier portion of the lower power phase (lower power
phase I) and the later portion (lower power phase II). In lower
power phase , no fuel was fed and combustion occurs in the
burn-out phase. This causes particle emissions to be significantly
different from that of lower power phase I. Particle number
concentrations were 4.8 10
7
particles/(N cm
3
) for the high
power phase, 5.8 10
6
particles/(N cm
3
) for lower power phase
, and 3.6 10
6
particles/(N cm
3
) for lower power phase .
Total particle number concentrations decreased significantly
along with the cooking procedure, which is correlated with the
rate of fuel burning and combustion condition. From Figure 4,
it can be observed that a prominent mode was less than 0.04
m, other than an accumulation mode peak near 0.20 m in
lower power phase , which suggests that particle number
emissions were largely in the nucleation mode. This observation
may be attributed to the lower particle number concentration
during lower power phase , which limited the condensation
and coagulation process and, hence, particle growth.
28,29
Although particle number concentrations and size distributions
varied to a certain extent in the repeated runs, a general trend
was found. The results of three repeated measurements of
particle emissions from stoves in Beijing were shown in Figure
5, and these indicated that the test data were satisfactorily
reproducible. Moreover, the relative standard deviation of the
particle average number concentration was less than 11%.
(26) Hueglin, Ch.; Gaegauf, Ch.; Kunzel, S.; Burtscher, H. EnViron. Sci.
Technol. 1997, 31, 3439-3447.
(27) Johansson, L. S.; Tullin, C.; Leckner, B.; Sjovall, P. Biomass
Bioenerg. 2003, 25, 435-436.
(28) Lipsky, E.; Stanier, C. O.; Pandis, S. P.; Robinson, A. L. Energy
Fuels 2000, 16, 302-310.
(29) Chang, M. C. O.; Chow, J. C.; Watson, J. G.; Hopke, P. K.; Yi, S.
M.; England, G. C. J. Air Waste Manage. Assoc. 2004, 54, 1494-1505.
Figure 3. Particle number concentration during the different phases
of the burning cycle.
Figure 4. Particle average number size distribution during the different
phases of the burning cycle.
Figure 5. Reproducibility of test data.
Figure 6. Particle mass size distribution of particles emitted from (a)
crop waste and (b) woody fuels combustion. (Note: SC, SH, and SB
denote the stoves in Chongqing, Henan, and Beijing , respectively.)
Emission Characteristics Household Biofuel Energy & Fuels, Vol. 21, No. 2, 2007 849
Particle Mass Size Distribution. Particle mass size distribu-
tions for all tested biofuel combustion during the whole burning
cycle, measured by LPI, are given in Figure 6. Particle mass
size distributions from crop waste combustion show a single
mode with the peak at approximately 0.20-0.48 m. However,
woody fuels show a bimodal size distribution; one prominent
mode peaks between 0.12 and 0.32 m, and the other weak
mode peaks at 0.76 m. It is supposed that soot contributes to
the mode at 0.76 m. A possible explanation is connected to
the fuel itself. Woody fuel has a higher lignin concentration
compared to the crop wastes. It was thought that a high lignin
concentration could increase the soot yield.
30
Unoxidized soot
may have undergone agglomeration and then growth to a
relatively large size. This needs to be further investigated. The
particle mass median aerodynamic diameter (MMD) is between
0.21 and 0.45 m. For all the biofuel combustion cases,
submicrometer particles (less than 1 m) contributed to over
90% of the mass of PM in the range of 0.03-2.39 m.
PM2.5 Emission. The emission factors of PM2.5 from rural
household biofuel combustion are between 1.80 and 7.00 g/kg
of biofuel (dry basis) and 0.84-2.40 g/MJ delivered energy;
the average emission factor is 4.21 g/kg of biofuel (dry basis)
and 1.46 g/MJ delivery energy for all of the biofuels tested
(Table 4). The results are consistent with previous studies.
13,31-33
The stove thermal efficiencies range from 13.4% to 22.1%.
The data are in accord with those measured from Chinese stoves
that burned biofuel in the laboratory.
15
Within that range, stoves
with different configurations have various thermal efficien-
cies: 13.4-16.1% for stoves in Chongqing, 18.0-22.1% for
stoves in Henan, and 14.8% for stoves in Beijing (Table 4).
The thermal efficiencies of the Henan stoves are generally
greater than the others. The stove in Henan has the least
combustion chamber volume, a grate, and the lowest distance
from the grate to the pot-bottom. All of those design features
contribute to high thermal efficiencies. However, the Henan
configuration can cause high emissions, described in the
following sections.
The mean emission factor of CO is between 29.3 and 134.0
g/kg of biofuel (dry basis) and 7.9-57.3 g/MJ delivered energy,
and the averaged value is 76.0 g/kg of biofuel (dry basis) and
29.4 g/MJ delivered energy over all the biofuel types tested
(Table 4). The results are also consistent with other re-
search.
11-13,15,32,34
PM2.5 emission factors in Henan are higher than those
measured in Beijing and Chongqing. This may be attributed to
different stove configurations. As mentioned above, the stove
in Henan has a small combustion volume, which leads to high
thermal efficiency, but the small volume may cause incomplete
combustion. Incomplete combustion of emitted organic matter
significantly enhances the formation of particles. The air supply
through the grate increases the temperature in the fuel bed and,
thereby, enhances vaporization of ash that would result in high
particle emissions.
35,36
Ash entrainment in the fuel bed escapes
to the flue gas as air flows through the grate. On the basis of
our findings, an increased thermal efficiency stove does not
imply reduced PM emissions (Figure 7). Other researchers also
reported this phenomenon.
11,13
Figure 8 shows the relationship between PM2.5 emission
factors on an energy basis and stove thermal efficiency, which
implies that the increase in thermal efficiency cannot offset the
increase in particle emissions.
(30) Wiinikka, H.; Gebart, R. Combust. Sci. Technol. 2005, 177, 741-
763.
(31) McDonald, J. D.; Zielinska, B.; Fujita, E. M.; Sagebiel, J. C.; Chow,
J. C. ; Waston, J. G. EnViron. Sci. Technol. 2000, 34, 2080-2091.
(32) Sheesley, R. J.; Schauer, J. J.; Chowdhury, Z.; Cass, G. R.; Simoneit,
E. R. T. Characterization of organic aerosols emitted from the combustion
of biomass indigenous to South Asia. J. Geophys. Res. 2003, 108 (D9),
4285; doi:10.109/2002JD002981.
(33) Fine, P. M.; Cass, G. R.; Simoneit, E. R. T. EnViron. Sci. Technol.
2001, 35, 2665-2675.
(34) Purious, C. R.; Mccrillis, R. C.; Kariher, P. H. EnViron. Sci. Technol.
2000, 34, 1653-1658.
(35) Jensen, P. A.; Frandsen, F. J.; Dam-Johansen, K.; Sander, B. Energy
Fuels 2000, 14, 1280-1285.
(36) Wiinikka, H. High temperature aerosol formation and emission
minimisation during combustion of wood pellets. Ph.D. Thesis, Technical
University of Denmark, Lyngby, Denmark, 2005.
Table 4. Thermal Efficiencies and Emission Factors of Biofuel Combustion
PM2.5 emission factors CO emission factors
stove fuel thermal efficiency (%) Em (g/kg)
a
Ee (g/MJ) Em (g/kg) Ee (g/MJ)
Chongqing rice straw 13.7 ( 1.1
b
1.66-1.94
c
0.79-0.90 108.9-128.6 51.9-59.5
maize residue 13.4 ( 1.0 2.45-3.85 1.03-1.68 111.5-156.5 48.5-66.1
bean straw 14.3 ( 0.9 3.28 ( 0.87 1.30 ( 0.35 77.0 ( 13.9 30.5 ( 5.5
fuel wood 16.1 ( 1.1 2.21-4.58 0.79-1.53 47.2-65.8 16.9-21.9
branch (I) 13.8 ( 1.1 2.95-3.97 1.17-1.58 62.7-93.3 24.8-37.1
Henan cotton stalk 18.7 ( 0.9 6.04 ( 0.52 1.75 ( 0.11 68.4 ( 23.8 19.7 ( 6.4
wheat residue 18.0 ( 0.9 5.61-8.39 1.86-2.94 62.5-68.7 21.9-22.7
kaoliang stalk 22.1 ( 0.7 6.27-7.19 1.63-2.02 27.9-30.7 7.3-8.6
Beijing branch (II) 14.8 ( 2.8
d
3.04 ( 0.85 1.11 ( 0.37 56.4 ( 22.6 20.4 ( 8.5
a
Dry fuel mass basis.
b
Three or more repeated tests, the results are given as means ( standard deviations (x ( s).
c
Two repeated tests, the results are
given as a range.
d
Just stove thermal efficiency, kang thermal efficiency is not included.
Figure 7. Relationship between stove thermal efficiency and PM2.5
emission factor on fuel mass basis. (Note: SC, SH, and SB denote the
stoves in Chongqing, Henan, and Beijing, respectively.)
850 Energy & Fuels, Vol. 21, No. 2, 2007 Li et al.
CO is a product of incomplete combustion. For low temper-
ature combustion in the household stove, organic matter emitted
from incomplete combustion enhances the formation of particles.
Gupta et al. found that CO emissions are correlated to those of
respirable suspended particulates (RSP).
37
However, in our
studies, a negative correlation between particle and CO emis-
sions was observed (Figure 9). Venkataraman et al. also found
opposing trends in PM and CO emissions in their study.
38
They
pointed out that CO emissions cannot be used as a surrogate
for PM emissions across stoves and fuels. This would indicate
that PM formation is complicated and needs to be studied
further.
Conclusions
The total average PM number concentrations for biofuel
combustion during the whole burning cycle was between 1.0
10
7
and 5.0 10
7
particles/(N cm
3
). Particle number size
distributions are mainly unimodal, with a peak between 0.12
and 0.32 m. In some cases, bimodal size distributions are also
observed, with a nucleation mode peak less than 0.04 m and
an accumulation mode peak near 0.12 m. Particle mass size
distributions from crop waste combustion show an obvious
single mode peak at 0.20-0.48 m; however, woody fuels show
a bimodal size distribution: one prominent mode peaks between
0.12 and 0.32 m, and the other weak mode peaks at 0.76 m.
Both with regard to number and mass, particle emissions from
biofuel combustion were dominated by submicrometer particles,
which imply adverse health concerns.
The emission factor of PM2.5 from biofuel combustion is
between 1.80 and 7.00 g/kg of biofuel (dry basis) and 0.84-
2.40 g/MJ delivered energy. The averages were 4.21 g/kg of
biofuel (dry basis) and 1.46 g/MJ delivered energy.
For household stoves, advanced gas cleaning devices are not
an economic option. The feasible way to reduce particle
emissions is, therefore, to decrease the formation of particles
in the combustion process. In this study, it appears that particle
emissions are correlated with combustion conditions and stove
configuration. Particle emissions are highest during the high
power phase. A possible way to reduce emissions in this phase
is by feeding the fuel at a moderate pace. Stove configuration
impacts both thermal efficiency and emissions. As noted, a
dilemma arises in that the more thermally efficient stove has
higher per kilogram fuel PM emissions and the increase in
thermal efficiency cannot offset the increase in particle emis-
sions. It is a stimulus for developing a stove with high efficiency
and low emissions.
Acknowledgment. The authors acknowledge the financial
support provided by the National Key Basic Research and Develop-
ment Program of China (Grant No. 2002CB211600) and the
National Natural Science Foundation of China (Grant No.
20521140077).
EF060150G
(37) Gupta, S.; Saksena, S.; Shankar, V. R.; Joshi, V. Biomass Bioenerg.
1998, 14, 547-559.
(38) Venkataraman, C.; Joshi, P.; Sethi, V.; Kohli, S.; Ravi, M. R. Aerosol
Sci. Tech. 2004, 38, 50-61.
Figure 8. Relationship between stove thermal efficiency and PM2.5
emission factor on energy basis. (Note: SC, SH, and SB denote the
stoves in Chongqing, Henan, and Beijing, respectively.)
Figure 9. Relationship between CO and PM2.5 emission factor.
Emission Characteristics Household Biofuel Energy & Fuels, Vol. 21, No. 2, 2007 851