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Letter

pubs.acs.org/journal/estlcu

Improving the Energy Eciency of Stoves To Reduce Pollutant


Emissions from Household Solid Fuel Combustion in China
Qing Li, Jingkun Jiang,*,, Juan Qi,, Jianguo Deng, Deshan Yang, Jianjun Wu,, Lei Duan,,
and Jiming Hao,#

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing
100084, China

State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing 100084, China

National Engineering Research Center of Coal Preparation and Purication, China University of Mining and Technology, Xuzhou
221116, China

Beijing Association of New Energy and Renewable Energy, Beijing 100029, China

School of Chemical Engineering and Technology, China University of Mining and Technology, Xuzhou 221116, China
#
Collaborative Innovation Centre for Regional Environmental Quality, Tsinghua University, Beijing 100084, China
S Supporting Information
*

ABSTRACT: Emissions of air pollutants from household solid fuel combustion in low-eciency
stoves have serious negative impacts on human health and air quality in China. This study compares
the thermal eciency (TE) and emissions from solid fuel combustion in a newly developed underre heating stove and a typical traditional over-re heating stove. The average TEs for burning all
tested fuel types (semi-coke, anthracite, briquette, bituminous, lignite, and biomass) were 83 and
42% for the new stove and the traditional stove, respectively. The new stove was eective in reducing
CO2 and pollutant emissions per unit energy delivered to a radiator. The average reductions were
50% for CO2, 79% for PM2.5, 95% for EC, 85% for benzo[a]pyrene equivalent carcinogenic
potency, and 66% for eight selected toxic elements (Pb, Cu, Sb, Cd, As, Ag, Se, and Ni) in PM2.5.
Improvements in stove technology are demonstrated as a practical approach for improving TE and
reducing emissions of hazardous pollutants and CO2.

diameter of 2.5 m) is greater than that of many industrial


sources, such as coal-red power plants.14
The TE of solid fuel burned in household stoves is lower
than that for fuel burned in industrial boilers. The TE of
traditional cookstoves in China was commonly less than 10%.15
Replacement stoves have been mainly designed with chimneys
to transport emissions from indoors to outdoors without a
signicant reduction in the total emission or improvement of
the TEs during the 1980s and 1990s.16,17 Rapid development of
stove technology has occurred in the past 15 years. The TE for
newly developed cookstoves, such as gasier cookstoves, was
increased to approximately 2735%.1820 The TE of heating
stoves promoted by Chinese local governments is commonly
lower than 55% according to our surveys, although their
claimed TE can be up to 6575%. The TE of household stoves
is mainly governed by two factors: heat transfer and
combustion eciencies. The heat transfer eciency is mainly
aected by the stove chamber structure. The combustion

INTRODUCTION
Coal is the dominant energy source in China and will continue
to be for a long time. Coal combustion makes the largest
contribution to ambient particulate matter (PM) pollution1 and
CO2 emissions2 in China. These emissions negatively impact
the global climate and human health.3,4 Considerable eort has
been spent to limit their emissions in China.59 Air pollution
control devices, such as electrostatic precipitators, desulfurization systems, and selective catalytic reduction, have been widely
installed on industrial coal boilers.6,911 There is another way
to think about driving down pollutant and CO2 emissions,11
i.e., improving the eciency of energy utilization. The designed
thermal eciency (TE) of Chinas industrial coal boilers is
currently 7280%, whereas the target set in Chinas 13th FiveYear Plan (20162020) is to exceed 90%. However, the
eciency of household stoves has attracted less interest from
the public and the government even though household solid
fuel combustion has been one of the major emission sources of
CO212 and air pollutants directly associated with negative
impacts on human health.13 More than 4 million people die
prematurely from illnesses that can be attributed to household
air pollution globally, and the contribution of household stoves
to atmospheric PM2.5 (particulate matter with an aerodynamic
XXXX American Chemical Society

Received: August 26, 2016


Revised: September 18, 2016
Accepted: September 19, 2016

DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. XXXX, XXX, XXXXXX

Letter

Environmental Science & Technology Letters

new stove is in pilot studies with some units deployed in the


Beijing area. Both stoves are operated by natural draft and
manual air controls. The internal space of the new stove can be
approximately divided into two chambers: a fuel storage
chamber and a secondary combustion chamber. The primary
combustion of solid fuel is red at the junction of the two
chambers, i.e., the bottom of the stove. Devolatilization occurs
in the lower part of the storage chamber because of the high
temperature in the combustion region. The carbonized solid
fuel is delivered by gravity feed, while the volatile gases are
drawn into the primary combustion region and then the
secondary combustion chamber by negative pressure. Additional air is supplied in the secondary combustion chamber to
further burn the volatile gases in the fuel gas. The surface area
for heat transfer to circulating water surrounds the pathway of
the ue gas. The traditional heating stove has only one
chamber, with the fuel batch placed in the bottom part of the
chamber. Fuel is fed into the chamber from the top to the
bottom and red from the bottom to the top with primary air
fed into the bottom. The upper fuel is carbonized and releases
the volatile gases when the bottom fuel is burning. The surface
area for heat transfer is mainly in the chamber walls and top
dust bae, which also has the function of capturing some dust
from the ue gas. Panels a and b of Figure S3 show
photographs of the two stoves tested, and panel c of Figure
S3 suggests that at the moment of fuel addition, the new stove
emits a level of pollutants considerably lower than that of the
traditional stove. The operational processes for the two stoves
are presented in the caption of Figure S3. Compared to the
traditional heating stove, the new stove has a relatively larger
water surface area because of its longer ue pathway (from the
stove bottom to the chimney). Along the ue pathway,
secondary air can be supplied to enhance the burning of
devolatilized matter.
Tested Fuel Samples. Six dierent types of solid fuel
samples were tested, including a semi-coke chunk (made from
bituminous coals with dimensions in the range of 0.34 cm),
anthracite chunk (37 cm), anthracite briquette (4 cm),
bituminous chunk (37 cm), lignite chunk (37 cm), and
biomass briquette (sphere-shaped, 4 cm) made from sawdust.
Table S1 presents the moisture, ash, volatile matter, xed
carbon, and sulfur contents, as well as net caloric value as
received, for the various fuels. Among these samples, semi-coke,
anthracite chunk, and anthracite briquette are considered as
promising potential clean fuels, whereas biomass was recently
recommended as a renewable fuel without net CO2 emissions.
Bituminous and lignite coals and raw biomass have been
recognized as dirty fuels because of their high volatile matter
content, which causes high PM emissions, but residential
consumers have preferred them because of their ease of ignition
and low price. These six samples were selected to represent six
types of solid fuels commonly used for household energy needs
in rural China.29
Tested Method and Sampling System. Combustion
experiments were conducted in the laboratory (see Figure S4)
for measuring emissions and TEs, while measurement of TEs
was also conducted in a household that has the traditional stove
and the new stove (see Figure S3). Five water-lled radiators
(for 150 m2 household heating) were connected in series to the
test stoves via a water circulating pump for both household and
laboratory testing. The fuel weight for each test was xed at
10.0 and 60.0 kg for the traditional and new stoves, respectively.
Three successful tests of full burning cycles (from ignition to

eciency in household stoves is commonly low and leads to


incomplete combustion. The incomplete combustion results in
larger emission factors (EFs) of PM and CO in residential
stoves than in industrial boilers.21 An estimated 36% of primary
PM2.5, 53% of elemental carbon (EC), and 62% of polycyclic
aromatic hydrocarbons (PAHs) in Chinas annual emissions are
from residential solid fuel combustion.18,2224 Residential solid
fuel combustion has led to serious air pollution with an increase
in environmental risk factors.13,2527 The replacement of raw
fuels with processed (or clean) fuel has been intensively
investigated as a way to reduce household air pollution. The
EFs of PM2.5, EC, organic carbon (OC), and PAHs for
anthracite coal and semi-coke briquette were reported to be
several dozen times lower than that for bituminous coal because
of the low volatile matter content,2831 whereas pelletized
biofuels and coal briquettes were reported to have low pollutant
EFs due to the change in their burning form.3236 However, in
some cases, cleaner fuels may not be eective for reducing the
emissions of CO2, toxic elements, or even PAHs.37,38
Additionally, the cleaner fuels are typically more expensive,
which in turn may result in residential consumers not choosing
them. In addition, specic stoves are often required for these
fuels, which are also a barrier for the deployment of new fuels as
residents may have to change their cooking and/or heating
habits. Since 2012, the Beijing government has launched a
policy of replacing all low-rank coals with anthracite with the
help of nancial subsidies, and Hebei province has planned the
replacement with 15 million tons of clean coal in 2016. These
policies require continuous and large amounts of nancial
support but have not yet made a considerable impact, as
illustrated by photographs in Figure S1, which show emissions
from typical residential solid fuel combustion in many areas in
China. According to the estimation of reduction scenarios
applied to the year 2010, cleaner stoves were proposed to
provide better emission reductions, even when free fuels are
used, compared to the deployment of cleaner fuels alone.16
However, there is little information about the in-use emission
and TE of updated cookstoves,1820 and there is no knowledge
of the performance of updated heating stoves.16 The new
household stoves should be based on updated combustion
technology and well-dened standards that include TE and
emissions of the most important pollutants, i.e., CO and PM2.5.
With the aim of improving TE and reducing pollutant EFs,
this study evaluates a newly developed heating stove that
employs under-re combustion technology, dierent from the
over-re technology commonly used in household stoves. The
technologies used in the new and traditional stoves are termed
under-re and over-re technologies according to the re
location in the stove chamber.39,40 Emissions from the
combustion of semi-coke, anthracite, coal briquette, bituminous, lignite, and biomass briquette samples in the new stove
are characterized and compared with those in a typical
traditional stove. The reductions in delivered energy-based
(based on useful energy delivered) CO2, PM2.5, OC, EC, PAH,
and selected toxic element EFs from the new stove are
presented, and the combustion technology aecting emissions
and TE is discussed.

MATERIALS AND METHODS


Tested Stoves and Combustion Technologies. Figure
S2 shows a schematic of the combustion technologies
employed by the two tested stoves. The tested traditional
stove is one of the most popular household coal stoves. The
B

DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. XXXX, XXX, XXXXXX

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Environmental Science & Technology Letters


re extinction) were conducted for each fuelstove combination in each laboratory test, while three more successful tests
were conducted for each combination in the household with
continuous operation for 24 h. Figure S4 shows a schematic of
the sampling system for measuring pollutant emissions and TEs
in the laboratory. The sampling system and calculation of
pollutant EFs have been previously described in detail and are
briey outlined here.30,31,41 The two stoves tested were placed
in a sealed room, and their ue gases mixed with dilution air
were drawn into a dilution tunnel. Possibly because of a higher
negative pressure above the stove chimney in the laboratory
testing and the resultant increase in combustion eciency, TEs
obtained under laboratory conditions are higher than those
obtained under household conditions (Table S2). However,
this dierence does not aect the comparison between the new
stove and the traditional stove when burning various fuels. All
pollutant concentrations were measured in the dilution tunnel.
A black carbon meter (Aethalometer, model AE 33, Magee
Scientic) was used to monitor the concentrations of ultraviolet
(370 nm)-absorbing PM and EC (880 nm) with diameters of
<2.5 m.42 The CO2 and CO, NOx, and SO2 concentrations
were measured by a CO2 meter (GC-0012, Gas Sensing
Solutions Ltd.) and active gas analyzers (models 48i, 43i, and
42i, Thermo Scientic), respectively. The modied combustion
eciency (MCE) was estimated as MCE = [CO2]/([CO2]
+ [CO]), where [CO2] and [CO] are the total molar
amounts of CO2 and CO, respectively, in the overall
combustion process.43,45 The total suspended particles
(TSPs) and PM2.5 were collected on lters using a fabricated
TSP sampler (10.0 L/min) and a PM2.5 cyclone (16.7 L/min,
URG-2000-30 EH, URG Inc.), respectively. PTFE membrane
and quartz-ber lters were used to collect PM during each
burning cycle. The PTFE membranes of collected PM2.5
samples were used to analyze eight toxic elements (Pb, Cu,
Sb, Cd, As, Ag, Se, and Ni) in the PM2.5 samples, and the quartz
membranes were used to analyze 16 priority PAHs (see the text
of the Supporting Information for the metal and PAH analysis
methods) and OC/EC in the PM2.5 samples. All obtained
values were used to directly calculate the corresponding massbased (based on the received mass of solid fuels) EFs. Using
the potency equivalency factor for individual PAHs relative to
benzo[a]pyrene (BaP), EFs of BaP equivalent carcinogenic
potency (BaPeq) were estimated to evaluate the cancer risk of
16 priority PAHs contained in PM2.5 samples.
The TE for each fuelstove combination was calculated as
TE = Qm/(MfQnet,ar), where Qm is the heating energy measured
by the calorimeter, Mf is the burned fuel mass in one testing
cycle, and Qnet,ar is the net caloric value of the burned fuel as
received. The calorimeter estimates Qm based on the water ow
rate and the temperature dierence between the water inlet and
outlet. Values of the calorimeter temperatures and ow rates
were calibrated during one combustion period by other
independent thermometers and owmeters, respectively. The
delivered energy-based EF (EFt) was obtained as EFt = EFm/
(TE Qnet,ar), where EFm is the mass-based EF.

Figure 1. (a) Thermal eciency, (b) modied combustion eciency,


and (c) average emission factors for solid fuel samples burned in
traditional and new stoves.

94%, was signicantly (p = 0.001) higher than that of the


traditional one, ranging from 24 to 56% (see Table S2). The
TEs obtained for the traditional stove correlated well with the
volatile matter contents of the fuels (p = 0.001), accounting for
97% of the variation in the TEs (see Figure S5). The average
MCEs for the new and traditional stoves were 96.5 1.8% and
92.8 3.6%, respectively. The MCEs for the traditional stove
also correlated well with the volatile matter contents of the fuels
(p = 0.05), accounting for 81% of the variation in the MCEs
(see Figure S5). The Students t test showed that the MCE for
the new stove was also signicantly (p = 0.05) higher than that
of the traditional one. Both the TE and the MCE for the new
stove did not show strong correlation with the volatile matter
content of the fuels (r = 0.3 for both). Thus, the new stove has
a considerably higher energy eciency regardless of the volatile
matter content of the fuel.
Emissions of CO2, PM, EC, BaPeq, and Eight Toxic
Elements. Delivered energy-based CO2 EFs were considerably
lower for the new stove than for the traditional stove because of
the considerably higher TE (see Figures 1c and 2). Because the
higher MCEs resulted in more complete combustion and
higher TE, both the mass- and delivered energy-based EFs of
CO, TSP, and PM2.5 were considerably lower for the new stove

RESULTS AND DISCUSSION


Thermal and Modied Combustion Eciencies. The
TE and MCE of all tested samples burned in the new stove
were higher than those in the traditional stove, as shown in
Figure 1. The average TEs for the new and traditional stoves
were 83 7% and 42 10%, respectively. A Students t test
showed that the TE for the new stove, ranging from 72 to
C

DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. XXXX, XXX, XXXXXX

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Environmental Science & Technology Letters

Figure 2. Reductions in the EFs of CO2, PM2.5, EC, BaPeq, and eight toxic elements when solid fuel samples are burned in the new stove in
comparison to the traditional stove.

(see Tables S3S6). Furthermore, the carbonaceous ratio in


PM2.5 was lower for the new stove, as were both the mass- and
delivered energy-based EFs of EC, BaPeq, and eight toxic
elements extracted from PM2.5 samples. Detailed data for both
mass- and delivered energy-based CO2 and pollutant EFs for all
tested samples in both stoves are listed in Tables S3S12. The
mass-based NO2 and SO2 EFs for the new stove were higher
than those for the traditional stove (see Table S3), possibly
because of the higher combustion eciency and burnout
ratio.30 However, the delivered energy-based NO2 and SO2 EFs
for most fuels are similar for both stoves.
Figure 2 summarizes the reductions in the delivered energybased EFs for CO2, PM2.5, EC, BaPeq, and eight toxic elements
caused by replacement of a tested traditional stove with a new
one. The average CO2 reduction, resulting from the improvement in TE, was 50 8%, with a range from 39 to 64%. The
average reductions in the EF of PM2.5 and its contents of EC,
BaPeq, and eight toxic elements were 79 18, 97 3, 85 15,
and 66 33%, respectively. The reductions in the EFs of PM2.5,
EC, BaPeq, and eight toxic elements for the three dirty fuels, i.e.,
bituminous, lignite, and biomass samples, were higher, with
average values of 95 3, 99.1 0.5, 97 3, and 95 1%,
respectively.
Volatile matter content in solid fuel not only governs PM2.5
EF from the traditional stove employing over-re technology
but also aects its TE and MCE. The over-re combustion
technology releases volatile matter from fuels without ecient
subsequent combustion when fuel is added to the stove
chamber. The unburnt volatile materials are precursors of
carbonaceous aerosols.44 Thus, particulate-bound pollutants are
mainly emitted during fuel ignition in the traditional stove,30 as
shown in Figure 3. After the pyrolysis stage, the emission rate of
volatile matter decreases with an increase in combustion time
and thus leads to a fast decrease in ultraviolet- and EC-channelabsorbing PM in the traditional stove.45 The under-re
combustion technology used in the new stove distills out the
volatile matter gradually, and the distilled volatile matter has a
higher combustion eciency because it passes through the
primary and secondary combustion regions (see Figures S2 and
S3). This improvement is supported by Figure 3, which shows
that the tested traditional stove had carbonaceous PM
emissions that were greater than those of the new stove after
the addition of the lignite coal. The combustion and emission
processes in the new stove are steadier without the highemission ignition stage.

Figure 3. Typical emission proles of ultraviolet (UV)- and ECchannel-absorbing particulate matter for the lignite coal burned in the
new and traditional stoves. These test samples were added to the
stoves before complete burnout of coals in their last cycles, and thus,
samples in both the new (20 kg) and traditional (10 kg) stove
chambers were ignited as if they were in practical use.

ENVIRONMENTAL IMPLICATIONS
The implication drawn from this study on household heating
stoves and studies of other gasier cookstoves tested in
China18,19,46 is that improving the energy and combustion
eciencies of household stoves is a practical approach to
alleviating the current pollutant situation and greatly improving
air quality. The superior performance of the new combustion
technology in reducing CO2 and PM emissions will reduce the
household contribution to atmospheric burden and indoor
health risks and save energy. Compared with the current
replacement with clean solid fuels annually in the Beijing
TianjingHebei region, the improvement in household stoves
is advantageous in terms of a lower cost with at least 10 years of
stove life and is more feasible than the deployment of clean
fuels, as the improvement policy can be more readily supervised
by the government. Additionally, the new stove appears to work
well for various solid fuels used in the residential sector of
China.
Considering the simplied assumption that the eciency of
all household stoves can be improved from the current value of
42 to 83% by employing the under-re combustion technology,
the mass of household solid fuel can be reduced by
approximately 49%. This would result in a potential savings
of approximately 50 Mt of coal, 90 Mt of rewood, and 130 Mt
of stalks in China based on estimates of their consumption in
D

DOI: 10.1021/acs.estlett.6b00324
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Environmental Science & Technology Letters


the past few years.41 Furthermore, reduction in emissions of
approximately 50% in CO2, 79% in PM2.5, and 95% in EC from
household combustion could also be realized. The reduction in
the emission of PAHs could lead to a reduction in the BaP
equivalent carcinogenic potency of 85%.

(7) Wu, X.; Yang, Q.; Chen, G.; Hayat, T.; Alsaedi, A. Progress and
prospect of CCS in China: Using learning curve to assess the costviability of a 2 600MW retrofitted oxyfuel power plant as a case
study. Renewable Sustainable Energy Rev. 2016, 60, 127485.
(8) Boot-Handford, M. E.; Abanades, J. C.; Anthony, E. J.; Blunt, M.
J.; Brandani, S.; Mac Dowell, N.; Fernandez, J. R.; Ferrari, M. C.;
Gross, R.; Hallett, J. P.; Haszeldine, R. S.; Heptonstall, P.; Lyngfelt, A.;
Makuch, Z.; Mangano, E.; Porter, R. T. J.; Pourkashanian, M.;
Rochelle, G. T.; Shah, N.; Yao, J. G.; Fennell, P. S. Carbon capture and
storage update. Energy Environ. Sci. 2014, 7 (1), 130189.
(9) Zhang, Q.; He, K. B.; Huo, H. Cleaning Chinas air. Nature 2012,
484 (7393), 161162.
(10) Xu, Y.; Williams, R. H.; Socolow, R. H. Chinas rapid
deployment of SO2 scrubbers. Energy Environ. Sci. 2009, 2 (5),
459465.
(11) You, C. F.; Xu, X. C. Coal combustion and its pollution control
in China. Energy 2010, 35 (11), 446772.
(12) Zhang, Y. X.; Wang, H. K.; Liang, S.; Xu, M.; Liu, W. D.; Li, S.
L.; Zhang, R. R.; Nielsen, C. P.; Bi, J. Temporal and spatial variations
in consumption-based carbon dioxide emissions in China. Renewable
Sustainable Energy Rev. 2014, 40, 6068.
(13) Zhang, J. J.; Smith, K. R. Household air pollution from coal and
biomass fuels in China: Measurements, health impacts, and
interventions. Environ. Health Persp 2007, 115 (6), 848855.
(14) Wang, S. X.; Zhao, B.; Cai, S. Y.; Klimont, Z.; Nielsen, C. P.;
Morikawa, T.; Woo, J. H.; Kim, Y.; Fu, X.; Xu, J. Y.; Hao, J. M.; He, K.
B. Emission trends and mitigation options for air pollutants in East
Asia. Atmos. Chem. Phys. 2014, 14 (13), 65716603.
(15) Sinton, J. E.; Smith, K. R.; Peabody, J. W.; Yaping, L.; Xiliang,
Z.; Edwards, R.; Quan, G. An assessment of programs to promote
improved household stoves in China. Energy Sustainable Dev. 2004, 8
(3), 3352.
(16) Winijkul, E.; Bond, T. C. Emissions from residential combustion
considering end-uses and spatial constraints: Part II, emission
reduction scenarios. Atmos. Environ. 2016, 124, 111.
(17) Smith, K. R.; Gu, S. H.; Huang, K.; Qiu, D. X. 100-Million
Improved Cookstoves In China - How Was It Done. World Dev 1993,
21 (6), 941961.
(18) Shen, G. F.; Chen, Y. C.; Xue, C. Y.; Lin, N.; Huang, Y.; Shen,
H. Z.; Wang, Y. L.; Li, T. C.; Zhang, Y. Y.; Su, S.; Huangfu, Y. B.;
Zhang, W. H.; Chen, X. F.; Liu, G. Q.; Liu, W. X.; Wang, X. L.; Wong,
M. H.; Tao, S. Pollutant Emissions from Improved Coal- and WoodFuelled Cookstoves in Rural Households. Environ. Sci. Technol. 2015,
49 (11), 659098.
(19) Carter, E. M.; Shan, M.; Yang, X. D.; Li, J. R.; Baumgartner, J.
Pollutant Emissions and Energy Efficiency of Chinese Gasifier
Cooking Stoves and Implications for Future Intervention Studies.
Environ. Sci. Technol. 2014, 48 (11), 646167.
(20) Panwar, N. L.; Rathore, N. S. Design and performance
evaluation of a 5 kW producer gas stove. Biomass Bioenergy 2008, 32
(12), 134952.
(21) Zhang, Y. X.; Schauer, J. J.; Zhang, Y. H.; Zeng, L. M.; Wei, Y. J.;
Liu, Y.; Shao, M. Characteristics of particulate carbon emissions from
real-world Chinese coal combustion. Environ. Sci. Technol. 2008, 42
(14), 506873.
(22) Huang, Y.; Shen, H. Z.; Chen, H.; Wang, R.; Zhang, Y. Y.; Su,
S.; Chen, Y. C.; Lin, N.; Zhuo, S. J.; Zhong, Q. R.; Wang, X. L.; Liu, J.
F.; Li, B. G.; Liu, W. X.; Tao, S. Quantification of Global Primary
Emissions of PM2.5, PM10, and TSP from Combustion and Industrial
Process Sources. Environ. Sci. Technol. 2014, 48 (23), 1383443.
(23) Shen, H. Z.; Huang, Y.; Wang, R.; Zhu, D.; Li, W.; Shen, G. F.;
Wang, B.; Zhang, Y. Y.; Chen, Y. C.; Lu, Y.; Chen, H.; Li, T. C.; Sun,
K.; Li, B. G.; Liu, W. X.; Liu, J. F.; Tao, S. Global Atmospheric
Emissions of Polycyclic Aromatic Hydrocarbons from 1960 to 2008
and Future Predictions. Environ. Sci. Technol. 2013, 47 (12), 641524.
(24) Wang, R.; Tao, S.; Wang, W. T.; Liu, J. F.; Shen, H. Z.; Shen, G.
F.; Wang, B.; Liu, X. P.; Li, W.; Huang, Y.; Zhang, Y. Y.; Lu, Y.; Chen,
H.; Chen, Y. C.; Wang, C.; Zhu, D.; Wang, X. L.; Li, B. G.; Liu, W. X.;

ASSOCIATED CONTENT

S Supporting Information
*

The Supporting Information is available free of charge on the


ACS Publications website at DOI: 10.1021/acs.estlett.6b00324.
Description of analysis methods for eight toxic elements
and 16 PAHs in PM2.5, fuel quality, values of TE and
MCE, mass- and delivered energy-based EFs of all
pollutant species cited in the main text, photographs of
polluted rural Beijing and tested stoves, stove technologies, the sampling system, and the relationship
between the TE and MCE and the fuel volatile matter
content (PDF)

AUTHOR INFORMATION

Corresponding Author

*Phone: +86-10-62781512. E-mail: jiangjk@tsinghua.edu.cn.


Notes

The authors declare no competing nancial interest.

ACKNOWLEDGMENTS
We thank Zizhen Ma from Tsinghua University and Lei Yu and
Dongfeng Liu from the China University of Mining and
Technology for their experimental support. Q.L. thanks Prof.
Yujing Mu from RCEES (CAS) for his helpful discussion.
Financial support from the National Key Basic Research and
Development Program of China (2013CB228505) and the
National Natural Science Foundation of China (41227805,
21422703, and 21521064) is acknowledged.

REFERENCES

(1) Duan, X. L.; Jiang, Y.; Wang, B. B.; Zhao, X. G.; Shen, G. F.; Cao,
S. Z.; Huang, N.; Qian, Y.; Chen, Y. T.; Wang, L. M. Household fuel
use for cooking and heating in China: Results from the first Chinese
Environmental Exposure-Related Human Activity Patterns Survey
(CEERHAPS). Appl. Energy 2014, 136, 692703.
(2) Liu, Z.; Guan, D. B.; Wei, W.; Davis, S. J.; Ciais, P.; Bai, J.; Peng,
S. S.; Zhang, Q.; Hubacek, K.; Marland, G.; Andres, R. J.; CrawfordBrown, D.; Lin, J. T.; Zhao, H. Y.; Hong, C. P.; Boden, T. A.; Feng, K.
S.; Peters, G. P.; Xi, F. M.; Liu, J. G.; Li, Y.; Zhao, Y.; Zeng, N.; He, K.
B. Reduced carbon emission estimates from fossil fuel combustion and
cement production in China. Nature 2015, 524 (7565), 335338.
(3) Bond, T. C.; Doherty, S. J.; Fahey, D. W.; Forster, P. M.;
Berntsen, T.; DeAngelo, B. J.; Flanner, M. G.; Ghan, S.; Karcher, B.;
Koch, D.; Kinne, S.; Kondo, Y.; Quinn, P. K.; Sarofim, M. C.; Schultz,
M. G.; Schulz, M.; Venkataraman, C.; Zhang, H.; Zhang, S.; Bellouin,
N.; Guttikunda, S. K.; Hopke, P. K.; Jacobson, M. Z.; Kaiser, J. W.;
Klimont, Z.; Lohmann, U.; Schwarz, J. P.; Shindell, D.; Storelvmo, T.;
Warren, S. G.; Zender, C. S. Bounding the role of black carbon in the
climate system: A scientific assessment. J. Geophys Res-Atmos 2013,
118 (11), 53805552.
(4) Lelieveld, J.; Evans, J. S.; Fnais, M.; Giannadaki, D.; Pozzer, A.
The contribution of outdoor air pollution sources to premature
mortality on a global scale. Nature 2015, 525 (7569), 367371.
(5) Wang, Q.; Liu, Q. L.; Shao, M.; Zhang, Y. H. Regional Air Quality
Management In China: A Case Study In the Pearl River Delta. Energy
Environ. 2013, 24 (78), 137392.
(6) Wang, S. X.; Hao, J. M. Air quality management in China: Issues,
challenges, and options. J. Environ. Sci. 2012, 24 (1), 213.
E

DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. XXXX, XXX, XXXXXX

Letter

Environmental Science & Technology Letters

Fired Hydronic Heaters. Environ. Sci. Technol. 2012, 46 (14), 7898


7904.
(41) Li, Q.; Jiang, J.; Cai, S.; Zhou, W.; Wang, S.; Duan, L.; Hao, J.
Gaseous Ammonia Emissions from Coal and Biomass Combustion in
Household Stoves with Different Combustion Efficiencies. Environ. Sci.
Technol. Lett. 2016, 3 (3), 98103.
(42) Kirchstetter, T. W.; Novakov, T.; Hobbs, P. V. Evidence that the
spectral dependence of light absorption by aerosols is affected by
organic carbon. J. Geophys Res-Atmos 2004, 109 (D21), D21208.
(43) Shen, G. F.; Yang, Y. F.; Wang, W.; Tao, S.; Zhu, C.; Min, Y. J.;
Xue, M. A.; Ding, J. N.; Wang, B.; Wang, R.; Shen, H. Z.; Li, W.;
Wang, X. L.; Russell, A. G. Emission Factors of Particulate Matter and
Elemental Carbon for Crop Residues and Coals Burned in Typical
Household Stoves in China. Environ. Sci. Technol. 2010, 44 (18),
715762.
(44) Wang, X. F.; Cotter, E.; Iyer, K. N.; Fang, J. X.; Williams, B. J.;
Biswas, P. Relationship between pyrolysis products and organic
aerosols formed during coal combustion. Proc. Combust. Inst. 2015, 35,
234754.
(45) Zhou, W.; Jiang, J.; Duan, L.; Hao, J. Evolution of
Submicrometer Organic Aerosols during a Complete Residential
Coal Combustion Process. Environ. Sci. Technol. 2016, 50 (14), 7861
7869.
(46) Sanford, L.; Burney, J. Cookstoves illustrate the need for a
comprehensive carbon market. Environ. Res. Lett. 2015, 10 (8),
08402636.

Ma, J. M. Black Carbon Emissions in China from 1949 to 2050.


Environ. Sci. Technol. 2012, 46 (14), 75957603.
(25) Smith, K. R.; Bruce, N.; Balakrishnan, K.; Adair-Rohani, H.;
Balmes, J.; Chafe, Z.; Dherani, M.; Hosgood, H. D.; Mehta, S.; Pope,
D.; Rehfuess, E. Millions Dead: How Do We Know and What Does It
Mean? Methods Used in the Comparative Risk Assessment of
Household Air Pollution. Annu. Rev. Public Health 2014, 35, 185206.
(26) Baumgartner, J.; Zhang, Y. X.; Schauer, J. J.; Huang, W.; Wang,
Y. Q.; Ezzati, M. Highway proximity and black carbon from cookstoves
as a risk factor for higher blood pressure in rural China. Proc. Natl.
Acad. Sci. U. S. A. 2014, 111 (36), 1322934.
(27) Rohra, H.; Taneja, A. Indoor air quality scenario in India-An
outline of household fuel combustion. Atmos. Environ. 2016, 129,
243255.
(28) Chen, Y. J.; Zhi, G. R.; Feng, Y. L.; Fu, J. M.; Feng, J. L.; Sheng,
G. Y.; Simoneit, B. R. T. Measurements of emission factors for primary
carbonaceous particles from residential raw-coal combustion in China.
Geophys. Res. Lett. 2006, 33 (20), L208158.
(29) Shen, G.; Xue, M.; Chen, Y.; Yang, C.; Li, W.; Shen, H.; Huang,
Y.; Zhang, Y.; Chen, H.; Zhu, Y.; Wu, H.; Ding, A.; Tao, S.
Comparison of carbonaceous particulate matter emission factors
among different solid fuels burned in residential stoves. Atmos. Environ.
2014, 89, 337345.
(30) Li, Q.; Li, X. H.; Jiang, J. K.; Duan, L.; Ge, S.; Zhang, Q.; Deng,
J. G.; Wang, S. X.; Hao, J. M. Semi-coke briquettes: towards reducing
emissions of primary PM2.5, particulate carbon, and carbon monoxide
from household coal combustion in China. Sci. Rep. 2016, 6, 19306
15.
(31) Li, Q.; Jiang, J.; Zhang, Q.; Zhou, W.; Cai, S.; Duan, L.; Ge, S.;
Hao, J. Influences of coal size, volatile matter content, and additive on
primary particulate matter emissions from household stove combustion. Fuel 2016, 182, 780787.
(32) Shen, G. F. Quantification of emission reduction potentials of
primary air pollutants from residential solid fuel combustion by
adopting cleaner fuels in China. J. Environ. Sci. 2015, 37, 17.
(33) Chen, Y.; Tian, C.; Feng, Y.; Zhi, G.; Li, J.; Zhang, G.
Measurements of emission factors of PM2.5, OC, EC, and BC for
household stoves of coal combustion in China. Atmos. Environ. 2015,
109, 190196.
(34) Bond, T. C.; Covert, D. S.; Kramlich, J. C.; Larson, T. V.;
Charlson, R. J. Primary particle emissions from residential coal
burning: Optical properties and size distributions. J. Geophys Res-Atmos
2002, 107 (D21), 83478355.
(35) Shen, G. F.; Tao, S.; Wei, S. Y.; Zhang, Y. Y.; Wang, R.; Wang,
B.; Li, W.; Shen, H. Z.; Huang, Y.; Chen, Y. C.; Chen, H.; Yang, Y. F.;
Wang, W.; Wei, W.; Wang, X. L.; Liu, W. X.; Wang, X. J.; Simonich, S.
L. M. Reductions in Emissions of Carbonaceous Particulate Matter
and Polycyclic Aromatic Hydrocarbons from Combustion of Biomass
Pellets in Comparison with Raw Fuel Burning. Environ. Sci. Technol.
2012, 46 (11), 640916.
(36) Shen, G. F. Changes from traditional solid fuels to clean
household energies - Opportunities in emission reduction of primary
PM2.5 from residential cookstoves in China. Biomass Bioenergy 2016,
86, 2835.
(37) Chen, Y. J.; Zhi, G. R.; Feng, Y. L.; Tian, C. G.; Bi, X. H.; Li, J.;
Zhang, G. Increase in polycyclic aromatic hydrocarbon (PAH)
emissions due to briquetting: A challenge to the coal briquetting
policy. Environ. Pollut. 2015, 204, 5863.
(38) Zhang, W.; Tong, Y. D.; Wang, H. H.; Chen, L.; Ou, L. B.;
Wang, X. J.; Liu, G. H.; Zhu, Y. Emission of Metals from Pelletized and
Uncompressed Biomass Fuels Combustion in Rural Household Stoves
in China. Sci. Rep. 2014, 4, 561116.
(39) Syc, M.; Horak, J.; Hopan, F.; Krpec, K.; Tomsej, T.; Ocelka, T.;
Pekarek, V. Effect of Fuels and Domestic Heating Appliance Types on
Emission Factors of Selected Organic Pollutants. Environ. Sci. Technol.
2011, 45 (21), 94279434.
(40) Aurell, J.; Gullett, B. K.; Tabor, D.; Touati, A.; Oudejans, L.
Semivolatile and Volatile Organic Compound Emissions from WoodF

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