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Letter

pubs.acs.org/journal/estlcu

Improving the Energy Efficiency 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 Purification, China University of Mining and Technology, Xuzhou
See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

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
Downloaded via 183.89.11.212 on January 2, 2024 at 16:06:19 (UTC).

*
S Supporting Information

ABSTRACT: Emissions of air pollutants from household solid fuel combustion in low-efficiency
stoves have serious negative impacts on human health and air quality in China. This study compares
the thermal efficiency (TE) and emissions from solid fuel combustion in a newly developed under-
fire heating stove and a typical traditional over-fire 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 effective 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.

■ INTRODUCTION
Coal is the dominant energy source in China and will continue
diameter of ≤2.5 μm) is greater than that of many industrial
sources, such as coal-fired power plants.14
to be for a long time. Coal combustion makes the largest The TE of solid fuel burned in household stoves is lower
contribution to ambient particulate matter (PM) pollution1 and than that for fuel burned in industrial boilers. The TE of
CO2 emissions2 in China. These emissions negatively impact traditional cookstoves in China was commonly less than 10%.15
the global climate and human health.3,4 Considerable effort has Replacement stoves have been mainly designed with chimneys
been spent to limit their emissions in China.5−9 Air pollution to transport emissions from indoors to outdoors without a
control devices, such as electrostatic precipitators, desulfuriza- significant reduction in the total emission or improvement of
tion systems, and selective catalytic reduction, have been widely the TEs during the 1980s and 1990s.16,17 Rapid development of
installed on industrial coal boilers.6,9−11 There is another way stove technology has occurred in the past 15 years. The TE for
to think about driving down pollutant and CO2 emissions,11 newly developed cookstoves, such as gasifier cookstoves, was
i.e., improving the efficiency of energy utilization. The designed increased to approximately 27−35%.18−20 The TE of heating
thermal efficiency (TE) of China’s industrial coal boilers is stoves promoted by Chinese local governments is commonly
currently 72−80%, whereas the target set in China’s 13th Five- lower than 55% according to our surveys, although their
Year Plan (2016−2020) is to exceed 90%. However, the claimed TE can be up to 65−75%. The TE of household stoves
efficiency of household stoves has attracted less interest from is mainly governed by two factors: heat transfer and
the public and the government even though household solid combustion efficiencies. The heat transfer efficiency is mainly
fuel combustion has been one of the major emission sources of affected by the stove chamber structure. The combustion
CO212 and air pollutants directly associated with negative
impacts on human health.13 More than 4 million people die Received: August 26, 2016
prematurely from illnesses that can be attributed to household Revised: September 18, 2016
air pollution globally, and the contribution of household stoves Accepted: September 19, 2016
to atmospheric PM2.5 (particulate matter with an aerodynamic Published: September 19, 2016

© 2016 American Chemical Society 369 DOI: 10.1021/acs.estlett.6b00324


Environ. Sci. Technol. Lett. 2016, 3, 369−374
Environmental Science & Technology Letters Letter

efficiency in household stoves is commonly low and leads to new stove is in pilot studies with some units deployed in the
incomplete combustion. The incomplete combustion results in Beijing area. Both stoves are operated by natural draft and
larger emission factors (EFs) of PM and CO in residential manual air controls. The internal space of the new stove can be
stoves than in industrial boilers.21 An estimated 36% of primary approximately divided into two chambers: a fuel storage
PM2.5, 53% of elemental carbon (EC), and 62% of polycyclic chamber and a secondary combustion chamber. The primary
aromatic hydrocarbons (PAHs) in China’s annual emissions are combustion of solid fuel is fired at the junction of the two
from residential solid fuel combustion.18,22−24 Residential solid chambers, i.e., the bottom of the stove. Devolatilization occurs
fuel combustion has led to serious air pollution with an increase in the lower part of the storage chamber because of the high
in environmental risk factors.13,25−27 The replacement of raw temperature in the combustion region. The carbonized solid
fuels with processed (or clean) fuel has been intensively fuel is delivered by gravity feed, while the volatile gases are
investigated as a way to reduce household air pollution. The drawn into the primary combustion region and then the
EFs of PM2.5, EC, organic carbon (OC), and PAHs for secondary combustion chamber by negative pressure. Addi-
anthracite coal and semi-coke briquette were reported to be tional air is supplied in the secondary combustion chamber to
several dozen times lower than that for bituminous coal because further burn the volatile gases in the fuel gas. The surface area
of the low volatile matter content,28−31 whereas pelletized for heat transfer to circulating water surrounds the pathway of
biofuels and coal briquettes were reported to have low pollutant the flue gas. The traditional heating stove has only one
EFs due to the change in their burning form.32−36 However, in chamber, with the fuel batch placed in the bottom part of the
some cases, cleaner fuels may not be effective for reducing the chamber. Fuel is fed into the chamber from the top to the
emissions of CO2, toxic elements, or even PAHs.37,38 bottom and fired from the bottom to the top with primary air
Additionally, the cleaner fuels are typically more expensive, fed into the bottom. The upper fuel is carbonized and releases
which in turn may result in residential consumers not choosing the volatile gases when the bottom fuel is burning. The surface
them. In addition, specific stoves are often required for these area for heat transfer is mainly in the chamber walls and top
fuels, which are also a barrier for the deployment of new fuels as dust baffle, which also has the function of capturing some dust
residents may have to change their cooking and/or heating from the flue gas. Panels a and b of Figure S3 show
habits. Since 2012, the Beijing government has launched a photographs of the two stoves tested, and panel c of Figure
policy of replacing all low-rank coals with anthracite with the S3 suggests that at the moment of fuel addition, the new stove
help of financial subsidies, and Hebei province has planned the emits a level of pollutants considerably lower than that of the
replacement with 15 million tons of clean coal in 2016. These traditional stove. The operational processes for the two stoves
policies require continuous and large amounts of financial are presented in the caption of Figure S3. Compared to the
support but have not yet made a considerable impact, as traditional heating stove, the new stove has a relatively larger
illustrated by photographs in Figure S1, which show emissions water surface area because of its longer flue pathway (from the
from typical residential solid fuel combustion in many areas in stove bottom to the chimney). Along the flue pathway,
China. According to the estimation of reduction scenarios secondary air can be supplied to enhance the burning of
applied to the year 2010, cleaner stoves were proposed to devolatilized matter.
provide better emission reductions, even when free fuels are Tested Fuel Samples. Six different types of solid fuel
used, compared to the deployment of cleaner fuels alone.16 samples were tested, including a semi-coke chunk (made from
However, there is little information about the in-use emission bituminous coals with dimensions in the range of 0.3−4 cm),
and TE of updated cookstoves,18−20 and there is no knowledge anthracite chunk (3−7 cm), anthracite briquette (∼4 cm),
of the performance of updated heating stoves.16 The new bituminous chunk (3−7 cm), lignite chunk (3−7 cm), and
household stoves should be based on updated combustion biomass briquette (sphere-shaped, ∼4 cm) made from sawdust.
technology and well-defined standards that include TE and Table S1 presents the moisture, ash, volatile matter, fixed
emissions of the most important pollutants, i.e., CO and PM2.5. carbon, and sulfur contents, as well as net calorific value as
With the aim of improving TE and reducing pollutant EFs, received, for the various fuels. Among these samples, semi-coke,
this study evaluates a newly developed heating stove that anthracite chunk, and anthracite briquette are considered as
employs under-fire combustion technology, different from the promising potential clean fuels, whereas biomass was recently
over-fire technology commonly used in household stoves. The recommended as a renewable fuel without net CO2 emissions.
technologies used in the new and traditional stoves are termed Bituminous and lignite coals and raw biomass have been
under-fire and over-fire technologies according to the fire recognized as dirty fuels because of their high volatile matter
location in the stove chamber.39,40 Emissions from the content, which causes high PM emissions, but residential
combustion of semi-coke, anthracite, coal briquette, bitumi- consumers have preferred them because of their ease of ignition
nous, lignite, and biomass briquette samples in the new stove and low price. These six samples were selected to represent six
are characterized and compared with those in a typical types of solid fuels commonly used for household energy needs
traditional stove. The reductions in delivered energy-based in rural China.29
(based on useful energy delivered) CO2, PM2.5, OC, EC, PAH, Tested Method and Sampling System. Combustion
and selected toxic element EFs from the new stove are experiments were conducted in the laboratory (see Figure S4)
presented, and the combustion technology affecting emissions for measuring emissions and TEs, while measurement of TEs
and TE is discussed.


was also conducted in a household that has the traditional stove
and the new stove (see Figure S3). Five water-filled radiators
MATERIALS AND METHODS (for 150 m2 household heating) were connected in series to the
Tested Stoves and Combustion Technologies. Figure test stoves via a water circulating pump for both household and
S2 shows a schematic of the combustion technologies laboratory testing. The fuel weight for each test was fixed at
employed by the two tested stoves. The tested traditional 10.0 and 60.0 kg for the traditional and new stoves, respectively.
stove is one of the most popular household coal stoves. The Three successful tests of full burning cycles (from ignition to
370 DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. 2016, 3, 369−374
Environmental Science & Technology Letters Letter

fire extinction) were conducted for each fuel−stove combina-


tion 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
briefly outlined here.30,31,41 The two stoves tested were placed
in a sealed room, and their flue 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 efficiency, TEs
obtained under laboratory conditions are higher than those
obtained under household conditions (Table S2). However,
this difference does not affect 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
Scientific) was used to monitor the concentrations of ultraviolet
(370 nm)-absorbing PM and EC (880 nm) with diameters of
<2.5 μm.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 Scientific), respectively. The modified combustion
efficiency (MCE) was estimated as MCE = Δ[CO2]/(Δ[CO2]
+ Δ[CO]), where Δ[CO2] and Δ[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 filters 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-fiber filters 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
Figure 1. (a) Thermal efficiency, (b) modified combustion efficiency,
methods) and OC/EC in the PM2.5 samples. All obtained and (c) average emission factors for solid fuel samples burned in
values were used to directly calculate the corresponding mass- traditional and new stoves.
based (based on the received mass of solid fuels) EFs. Using
the potency equivalency factor for individual PAHs relative to ∼94%, was significantly (p = 0.001) higher than that of the
benzo[a]pyrene (BaP), EFs of BaP equivalent carcinogenic traditional one, ranging from ∼24 to ∼56% (see Table S2). The
potency (BaPeq) were estimated to evaluate the cancer risk of TEs obtained for the traditional stove correlated well with the
16 priority PAHs contained in PM2.5 samples. volatile matter contents of the fuels (p = 0.001), accounting for
The TE for each fuel−stove combination was calculated as 97% of the variation in the TEs (see Figure S5). The average
TE = Qm/(MfQnet,ar), where Qm is the heating energy measured MCEs for the new and traditional stoves were 96.5 ± 1.8% and
by the calorimeter, Mf is the burned fuel mass in one testing 92.8 ± 3.6%, respectively. The MCEs for the traditional stove
cycle, and Qnet,ar is the net calorific value of the burned fuel as also correlated well with the volatile matter contents of the fuels
received. The calorimeter estimates Qm based on the water flow (p = 0.05), accounting for 81% of the variation in the MCEs
rate and the temperature difference between the water inlet and (see Figure S5). The Student’s t test showed that the MCE for
outlet. Values of the calorimeter temperatures and flow rates the new stove was also significantly (p = 0.05) higher than that
were calibrated during one combustion period by other of the traditional one. Both the TE and the MCE for the new
independent thermometers and flowmeters, respectively. The stove did not show strong correlation with the volatile matter
delivered energy-based EF (EFt) was obtained as EFt = EFm/ content of the fuels (r = 0.3 for both). Thus, the new stove has
(TE × Qnet,ar), where EFm is the mass-based EF.


a considerably higher energy efficiency regardless of the volatile
matter content of the fuel.
RESULTS AND DISCUSSION Emissions of CO2, PM, EC, BaPeq, and Eight Toxic
Thermal and Modified Combustion Efficiencies. The Elements. Delivered energy-based CO2 EFs were considerably
TE and MCE of all tested samples burned in the new stove lower for the new stove than for the traditional stove because of
were higher than those in the traditional stove, as shown in the considerably higher TE (see Figures 1c and 2). Because the
Figure 1. The average TEs for the new and traditional stoves higher MCEs resulted in more complete combustion and
were 83 ± 7% and 42 ± 10%, respectively. A Student’s t test higher TE, both the mass- and delivered energy-based EFs of
showed that the TE for the new stove, ranging from ∼72 to CO, TSP, and PM2.5 were considerably lower for the new stove
371 DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. 2016, 3, 369−374
Environmental Science & Technology Letters Letter

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 S3−S6). 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 S3−S12. 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 efficiency 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 energy-
based 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 improve- Figure 3. Typical emission profiles of ultraviolet (UV)- and EC-
ment in TE, was 50 ± 8%, with a range from 39 to 64%. The channel-absorbing particulate matter for the lignite coal burned in the
new and traditional stoves. These test samples were added to the
average reductions in the EF of PM2.5 and its contents of EC,
stoves before complete burnout of coals in their last cycles, and thus,
BaPeq, and eight toxic elements were 79 ± 18, 97 ± 3, 85 ± 15, samples in both the new (20 kg) and traditional (10 kg) stove
and 66 ± 33%, respectively. The reductions in the EFs of PM2.5, chambers were ignited as if they were in practical use.


EC, BaPeq, and eight toxic elements for the three dirty fuels, i.e.,
bituminous, lignite, and biomass samples, were higher, with ENVIRONMENTAL IMPLICATIONS
average values of 95 ± 3, 99.1 ± 0.5, 97 ± 3, and 95 ± 1%,
respectively. The implication drawn from this study on household heating
Volatile matter content in solid fuel not only governs PM2.5 stoves and studies of other gasifier cookstoves tested in
EF from the traditional stove employing over-fire technology China18,19,46 is that improving the energy and combustion
but also affects its TE and MCE. The over-fire combustion efficiencies of household stoves is a practical approach to
technology releases volatile matter from fuels without efficient alleviating the current pollutant situation and greatly improving
air quality. The superior performance of the new combustion
subsequent combustion when fuel is added to the stove
technology in reducing CO2 and PM emissions will reduce the
chamber. The unburnt volatile materials are precursors of
household contribution to atmospheric burden and indoor
carbonaceous aerosols.44 Thus, particulate-bound pollutants are
health risks and save energy. Compared with the current
mainly emitted during fuel ignition in the traditional stove,30 as replacement with clean solid fuels annually in the Beijing−
shown in Figure 3. After the pyrolysis stage, the emission rate of Tianjing−Hebei region, the improvement in household stoves
volatile matter decreases with an increase in combustion time is advantageous in terms of a lower cost with at least 10 years of
and thus leads to a fast decrease in ultraviolet- and EC-channel- stove life and is more feasible than the deployment of clean
absorbing PM in the traditional stove.45 The under-fire fuels, as the improvement policy can be more readily supervised
combustion technology used in the new stove distills out the by the government. Additionally, the new stove appears to work
volatile matter gradually, and the distilled volatile matter has a well for various solid fuels used in the residential sector of
higher combustion efficiency because it passes through the China.
primary and secondary combustion regions (see Figures S2 and Considering the simplified assumption that the efficiency of
S3). This improvement is supported by Figure 3, which shows all household stoves can be improved from the current value of
that the tested traditional stove had carbonaceous PM 42 to 83% by employing the under-fire combustion technology,
emissions that were greater than those of the new stove after the mass of household solid fuel can be reduced by
the addition of the lignite coal. The combustion and emission approximately 49%. This would result in a potential savings
processes in the new stove are steadier without the high- of approximately 50 Mt of coal, 90 Mt of firewood, and 130 Mt
emission ignition stage. of stalks in China based on estimates of their consumption in
372 DOI: 10.1021/acs.estlett.6b00324
Environ. Sci. Technol. Lett. 2016, 3, 369−374
Environmental Science & Technology Letters Letter

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biomass fuels in China: Measurements, health impacts, and
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*Phone: +86-10-62781512. E-mail: jiangjk@tsinghua.edu.cn. (14) Wang, S. X.; Zhao, B.; Cai, S. Y.; Klimont, Z.; Nielsen, C. P.;
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Z.; Edwards, R.; Quan, G. An assessment of programs to promote
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Dongfeng Liu from the China University of Mining and (3), 33−52.
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Development Program of China (2013CB228505) and the (17) Smith, K. R.; Gu, S. H.; Huang, K.; Qiu, D. X. 100-Million
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374 DOI: 10.1021/acs.estlett.6b00324


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