Evolution of Ozone Formation Sensitivity during a Persistent Regional Ozone Episode in Northeastern China and Its Implication for a Control Strategy.

In recent years, the magnitude and frequency of regional ozone (O3) episodes have increased in China. We combined ground-based measurements, observation-based model (OBM), and the Weather Research and Forecasting and Community Multiscale Air Quality (WRF-CMAQ) model to analyze a typical persistent O3 episode that occurred across 88 cities in northeastern China during June 19-30, 2021. The meteorological conditions, particularly the wind convergence centers, played crucial roles in the evolution of O3 pollution. Daily analysis of the O3 formation sensitivity showed that O3 formation was in the volatile organic compound (VOC)-limited or transitional regime at the onset of the pollution episode in 92% of the cities. Conversely, it tended to be or eventually became a NOx-limited regime as the episode progressed in the most polluted cities. Based on the emission-reduction scenario simulations, mitigation of the regional O3 pollution was found to be most effective through a phased control strategy, namely, reduction of a high ratio of VOCs to NOx at the onset of the pollution and lower ratio during evolution of the O3 episode. This study presents a new possibility for regional O3 pollution abatement in China based on a reasonable combination of OBM and the WRF-CMAQ model.

Investigating the relationship between mass concentration of particulate matter and reactive oxygen species based on residential coal combustion source tests.

Particulate matter (PM) has been considered to be closely related to human health, especially fine particulate matter. However, whether PM mass concentration alone is a good indicator for health impact remains a challenging question. In this study, emissions from residential coal combustion (RCC), one of the important PM sources in northern China, were tested to examine the relationship between the emission factors of particle-generated reactive oxygen species (ROS) (EFROS) and PM (EFPM). A total of 24 combinations of source tests were conducted, including eight types of coal with different geological maturities (two anthracites and six bituminous) burned in three types of stoves (one honeycomb coal stove, one old chunk stove, and one new chunk stove). Here, ROS was defined as generated hydroxyl radical (·OH) by PM, and results showed EFROS from 24 residential coal combustion varied greatly by nearly 20 times. EFROS ranged 0.78-14.85 and 2.99-12.91 mg kg-1 for the emissions from honeycomb and chunk coals, respectively. Moreover, the correlation between EFROS and EFPM was significantly positive in honeycomb coal emissions (r = 0.82, p < 0.05), but it was insignificant in chunk coal emissions (r = 0.07, p > 0.05). For honeycomb coal emissions, organic carbon (OC) was quite abundant in PM and it might be the predominant contributor to both EFPM and EFROS, resulting in a strong and positive correlation. For chunk coal emissions, high EFROS was mainly related to relatively high metal emissions in AN and LVB, while the metals were not major components in PM, leading to a poor correlation between EFPM and EFROS. Therefore, this study revealed that PM was not always positively correlated with ROS from residential coal burning, and the relationship was mainly determined by the compositions of PM, suggesting PM mass concentration alone may not be the best indicator for assessing health impacts.

A preliminary study on pollution characteristics of surfactant substances in fine particles in the Beibu Gulf Region of China.

The pollution characteristics of surfactant substances in fine particles (PM2.5) in spring were studied in the Beibu Gulf Region of China, 68 samples of PM2.5 were collected at Weizhou Island in Beihai City from March 12 to April 17, 2015. The Anionic Surfactant Substances (ASS) and Cationic Surfactant Substances (CSS) in the samples were analyzed using Byethyl Violet Spectrophotometry and Disulfide Blue Spectrophotometry, respectively. Combined with the data from backward trajectory simulation, the effects of air pollutants from remote transport on the pollution characteristics of surfactant substances in PM2.5 in the Beibu Gulf Region were analyzed and discussed. The results showed that the daily mean concentrations of ASS and CSS in spring in the Beibu Gulf Region were 165.20 pmol/m3 and 8.05pmol/m3, and the variation ranges were 23.21-452.55 pmol/m3 and 0.65-31.31 pmol/m3, accounting for 1.82‰ ± 1.65‰ and 0.12‰ ± 0.11‰ of the mass concentration of PM2.5, respectively. These concentrations were lower than those in comparable regions around the world. There was no clear correlation between the concentrations of ASS and CSS in PM2.5 and the mass concentrations of PM2.5. Tourism and air transport had a positive contribution on the concentrations of ASS. The concentration of surfactant substances in PM2.5 was significantly impacted by wind speed and wind direction. Atmospheric temperature, air pressure and precipitation had little effect on the concentrations of surfactant substances. Surfactant substances in PM2.5 significantly impacted visibility. Results also showed that the main sources of surfactant substances were from the southern China and Southeast Asia.

Comparison of elemental and black carbon measurements during normal and heavy haze periods: implications for research.

Studies specifically addressing the elemental carbon (EC)/black carbon (BC) relationship during the transition from clean-normal (CN) air quality to heavy haze (HH) are rare but have important health and climate implications. The present study, in which EC levels are measured using a thermal-optical method and BC levels are measured using an optical method (aethalometer), provides a preliminary insight into this issue. The average daily EC concentration was 3.08 ± 1.10 µg/m(3) during the CN stage but climbed to 11.77 ± 2.01 µg/m(3) during the HH stage. More importantly, the BC/EC ratio averaged 0.92 ± 0.14 during the CN state and increased to 1.88 ± 0.30 during the HH state. This significant increase in BC/EC ratio has been confirmed to result partially from an increase in the in situ light absorption efficiency (σap) due to an enhanced internal mixing of the EC with other species. However, the exact enhancement of σap was unavailable because our monitoring scheme could not acquire the in situ absorption (bap) essential for σap calculation. This reveals a need to perform simultaneous measurement of EC and bap over a time period that includes both the CN and HH stages. In addition, the sensitivity of EC to both anthropogenic emissions and HH conditions implies a need to systematically study how to include EC complex (EC concentration, OC/EC ratio, and σap) as an indicator in air quality observations, in alert systems that assess air quality, and in the governance of emissions and human behaviors.

A review of quantification methods for light absorption enhancement of black carbon aerosol.

Black carbon (BC) is a distinct type of carbonaceous aerosol that has a significant impact on the environment, human health, and climate. A non-BC material coating on BC can alter the mixing state of the BC particles, which considerably enhances the mass absorption efficiency of BC by directing more energy toward the BC cores (lensing effect). A lot of methods have been reported for quantifying the enhancement factor (Eabs), with diverse results. However, to the best of our knowledge, a comprehensive review specific to the quantification methods for Eabs has not been systematically performed, which is unfavorable for the evaluation of obtained results and subsequent radiative forcing. In this review, quantification methods are divided into two broad categories, direct and indirect, depending on whether experimental removal of the coating layer from an aged carbonaceous particle is required. The direct methods described include thermal peeling, solvent dissolution, and optical virtual exfoliation, while the indirect methods include intercept-linear regression fitting, minimum R squared, numerical simulation, and empirical value. We summarized the principles, procedures, virtues, and limitations of the major Eabs quantification methods and analyzed the current problems in the determination of Eabs. We pointed out what breakthroughs are needed to improve or innovate Eabs quantification methods, particularly regarding the need to avoid the influence of brown carbon, develop a broadband Eabs quantification scheme, quantify the Eabs values for the emissions of low-efficiency combustions, measure the Eabs of particles in a high-humidity environment, design a real-time monitor of Eabs by a proper combination of mature techniques, and make more use of artificial intelligence for better Eabs quantification. This review deepens the understanding of Eabs quantification methods and benefits the estimation of the contribution of BC to radiative forcing using climate models.

The integrating sphere system plus in-situ absorption monitoring: A new scheme to study absorption enhancement of black carbon in ambient aerosols.

Black carbon (BC) is the strongest light-absorbing aerosol in the atmosphere. The coating process causes lensing effects to enhance the BC absorption. The reported BC absorption enhancement values (Eabs) significantly differ partly due to the measurement methods used. The biggest difficulty in measuring the Eabs values is how to denude the coated particles so that the true value of absorption without coatings can be distinguished from lensing effects. In this study, we proposed a new approach based on an integrating sphere (IS) system plus in-situ absorption monitoring instrument to study Eabs in ambient aerosols. This approach is capable of (i) "de-lensing through solvent dissolution and solvent de-refraction", by which the absorption coefficient of denuded BC is acquired, and (ii) monitoring in-situ absorption with photoacoustic spectroscopy. With the help of the EC concentration measured by a thermal/optical carbon analyser, the Eabs values were calculated as the quotient of in-situ mass absorption efficiency divided by denude mass absorption efficiency. We applied this new approach to measure the Eabs values of four seasons in Beijing and found an annual mean of 1.90 ± 0.41 in 2019. More importantly, a previous assumption that BC absorption efficiency may be progressively enhanced by increased air pollution was validated and quantified using a logarithmic relationship of Eabs = 0.6 ln (PM2.5 ̶ 3.59) ̶ 0.43 (R2 = 0.99). This signals a continued drop of Eabs for future ambient aerosols with the sustained improvement in local air quality in China, meriting serious attention to its influences in climate, air quality, and atmospheric chemistry.

Identifying the fundamental drives behind the 10-year evolution of northern China's rural household energy and emission: Implications for 2030 and beyond.

Rural household energy, particularly solid fuels, in northern China is thought to be a major source of air pollution. However, there is no complete, systematic, and reliable dataset for northern China's rural areas owing to the diversity of energy types used and the difficulty in acquiring data, particularly for solid fuels. Here we assessed existing progress in estimating solid fuels and proposed a practical route for deriving the information on rural household energy consumption and structure in northern China spanning 2010-2020, with important findings. (i) In 2010, the total rural household energy consumption for northern China was 287.51 million tons standard coal equivalent (TCE), while for 2020, it decreased to 205.14 million TCE, showing a 29 % decrease and an annual down 3.3 % averagely. Among a number of underlying reasons, China's urbanization process, which made the rural population shrink year by year, was primarily responsible. (ii) The share of clean energy in northern rural areas began at 4.2 % in 2010 and grew to 15.6 % in 2020, displaying a sustained improvement in energy structure. Particularly in the second 5 years, the clean energy share of policy priority areas grew by 20.0 percentage points (from 15.0 % in 2010 to 35.0 % in 2020), which is more than 18 percentage points higher than the growth of non-priority areas (from 2.9 % in 2010 to 4.5 % in 2020). Clean air policy, particularly the "two replacements" (replace coal with gas and electricity), in priority areas played a core role in changing the energy structure. (iii) Although both air pollutants and CO2 are predicted to decrease in 2030, there is a large gap between expected 2030 emissions and hoped 2060 carbon neutrality in northern rural households. It is thus necessary to gradually boost the share of green electricity (non-fossil) and to reverse the trend of "biomass fuel curtailment" in rural residential sector. This calls for the improvement in biomass style (e.g., biomass pellets) and in stove efficiency (e.g., complete combustion).

Harmonizing aerosol carbon measurements between two conventional thermal/optical analysis methods.

Although total carbon (TC) can be consistently quantified by various aerosol carbon measurement methods, the demarcation of TC into organic carbon (OC) and elemental carbon (EC) has long been inconsistent. The NIOSH and IMPROVE protocols are most widely used for thermal/optical analysis (TOA), but current knowledge rests in the description that the NIOSH protocol usually gives lower EC values than does the IMPROVE protocol. This study seeks to explore the possibility of quantitatively linking the difference between the two TOA protocols. Residential coal-burning samples that had been collected and analyzed following the NIOSH protocol in previous studies were directly reanalyzed following the IMPROVE protocol for this study. A comparison of each pair of NIOSH and IMPROVE EC values reveals the dynamic relation between the two protocols, which can be expressed as a regression equation, y=(1-x)/(1+4.86x2) (R2=0.96), where the independent x is the EC/TC ratio R(EC/TC) for the IMPROVE protocol, and the dependent y is the difference between IMPROVE and NIOSH REC/TC relative to IMPROVE REC/TC. This regression equation may be the first effort in formulating the relationship between the two TOA protocols, and it is very helpful in harmonizing inconsistent TOA measurements, for example, source characterization, ambient monitoring, and atmospheric modeling.

Toward a national emission inventory for the catering industry in China.

Catering oil fumes are a major hazard to human health. In particular, the typical Chinese cooking style is characterised by a high temperature frying process that produces high levels of cooking oil fumes. However, limited data relating to this sector mean that national emission inventory data specific to the catering service industry do not exist. To address above deficiency and thus to establish the inventory of a city, or a province, or even a country, a door-to-door survey campaign was launched in the Chinese cities of Heze and Linfen to determine the structure of local catering industries. Data revealed that the number of catering businesses per 104 people was 17 ± 4. Of these, 3.0 ± 1.4, 15.0 ± 1.4, and 82.0 ± 0.0% were classified as large, medium, and small enterprises, respectively. Furthermore, the installation rates of fume purifiers were 74 ± 13, 66 ± 9, and 51 ± 14% for large, medium, and small enterprises, respectively, with net removal efficiencies of 63 ± 11, 50 ± 7, and 31 ± 8%, respectively. This information was extrapolated across all provincial regions of China to construct a provincial and national emission inventory. In 2017, China's national catering industry released approximately 34 kt of volatile organic compounds (VOCs), 38 kt of particulate matter with a diameter less than 2.5 µm (PM2.5), 48 kt of particulate matter with a diameter less than 10 µm (PM10), 1 kt of black carbon (BC), and 27 kt of organic carbon (OC). A significant correlation was observed between vegetable oil consumption and emissions (e.g., for VOCs, y = 14.94 x + 76.50, R2 = 0.87, where y is VOCs emissions and x is vegetable oil consumption), indirectly corroborating the rationality of the inventory. Moreover, this correlation provides the potential for a dynamic inventory based on vegetable oil consumption. Future studies are proposed to address more influential factors to improve the reliability of the national inventory and refer to big data, rather than door-to-door investigation, to identify the amount of catering service businesses in a region.

Algorithm developed for dynamic quantification of coal consumption for and emission from rural winter heating.

Coal-dominated winter heating practices in China are largely accepted to be a leading cause of winter haze in the region though the amount of coal for heating is actually much lower than for power generation or industrial process. However, little is known about how the total rural coal weight in a region could be attributed to real time (e.g., daily) patterns, limiting the understanding of dynamic impacts of coal emissions and the adoption of timely measures against predicted haze. Considering that winter heating essentially protects against cold temperatures, coal burning strength may be related to the temperatures that people experience. A field study was organized to test the validity of this hypothesis. A system was designed to continuously monitor every instance of coal addition, and coal consumption on any given day for a whole village (WDAY) was calculated by summating all the additions. Meanwhile, a new term, composite temperature (TCOM), which incorporates a few weather-related elements, was introduced to represent cold temperatures that individuals experience. It was found that WDAY and TCOM presented opposite variations, and a negative linear correlation was observed (WDAY = -0.75TCOM + 11.86, R2 = 0.75), revealing the feasibility of estimating coal consumption on a certain day (WDAY) based on weather data (TCOM) for a given village. An extensive form of the algorithm for any area of interest (e.g., a district, city, or province) can be expressed as WDAY = (-0.75TCOM + 11.86)‧NH/834, where NH denotes the number of households in a region. This algorithm reflects the essence of winter heating (to resist cold temperatures), and therefore its logic is highly likely to be useful for any countries of the world regardless of what forms of energy used (coal or other energy forms) provided the energy involved is unexceptionally used for winter heating, though there may be some uncertainties in estimated coal consumption due to multiple factors.

Effects of temperature parameters on thermal-optical analysis of organic and elemental carbon in aerosol.

Thermal-optical analysis (TOA) is a popular method to determine aerosol elemental carbon (EC) and organic carbon (OC) collected on quartz fiber filter. However, temperature protocol adopted in TOA has great effects on OC and EC results. The purpose of this study is to investigate and quantify the effects of maximum temperature (T(max)) and residence time (RT) for each step in helium stage on ECOC measurements. Fourteen typical source samples and 20 ambient samples were collected and six temperature programs were designed for this study. It was found that EC value decreases regularly as T(max ) ascends, i.e., EC results from T(max) of 650 degrees C, 750 degrees C and 850 degrees C are 0.89 +/- 0.06, 0.76 +/- 0.10, 0.62 +/- 0.13 times EC value from T( max) of 550 degrees C, respectively, and the magnitude of EC drop (EC(d), percent) is significantly correlated with OC abundance in total carbon (R(OC/TC)), expressed as EC(d) = 66.8R(OC/TC)-14.4 (r = 0.87); pyrolized OC(POC) values are also sensitive to T(max), but there are various trends for samples with different OC constituents. On average of the samples studied here, prolonged RT reduces EC values by only 3%, almost negligible compared to the effect of T(max), and reduces POC by 9%, much less than that by previous report.

[Characteristics of Heavy Metal Pollutants of PM2.5 from Open Burning of Municipal Solid Waste (MSW) and the Associated Exposure Health Risks].

The characteristics and health risk assessment for heavy metal pollutants in PM2.5 discharged from the open burning of municipal solid waste (MSW) in different functional areas were studied using a flue gas diluted sampling system. The two common open burning modes of barrel and natural pile-up burning were considered. The results show that the concentration of zinc (Zn) was the highest among the heavy metals produced by five different components of waste incineration, ranging from 1324.03 to 3703.12 mg·kg-1. The concentration of cadmium (Cd) was the lowest, ranging from 20.25 to 63.68 mg·kg-1. According to the geo-accumulation index, lead (Pb), Zn, arsenic (As), and Cd were highly polluted in the measured MSW samples, and all four of these metals reached moderate or higher levels of pollution under natural pile-up burning methods. The geo-accumulation index of Cd was much higher than 5. The results of the human health risk assessment showed that non-carcinogenic risk values for 8 heavy metals (Pb, Zn, Cu, Mn, As, Cd, Cr, and Ni) by respiratory exposure were less than 1, which is within the safe range. For natural pile-up burning, the total non-carcinogenic risk values for As and Pb for children were higher than 1, indicating a non-carcinogenic risk. The carcinogenic risk values for four carcinogenic elements (As, Cd, Cr, and Ni) were less than 1.0×10-4, but still represented a low potential carcinogenic risk under exposure for long periods of time.

[Emission Characteristics and Chemical Components of PM2.5 from Open Burning of Municipal Solid Waste].

Source emission measurements were employed to investigate open burning of municipal solid waste (MSW). Both barrel and natural pile-up burning of MSW were investigated using a self-designed dilution sampling system. PM2.5 was collected for three types of waste, including rubber and plastic, paper, and wood and bamboo. Then, components in the samples were analyzed and emission factors of PM2.5, organic carbon (OC), elemental carbon (EC), water-soluble ions and inorganic elements were calculated. The PM2.5 emission factor was highest for wood and bamboo, and lowest for paper, and was calculated to be (7.44±0.76) g·kg-1 and (2.72±0.52) g·kg-1, respectively. Barrel burning resulted in much higher pollutant emissions. The PM2.5 emission factor for barrel burning was 2.5-3.5 times that of natural pile-up burning. OC and EC were the main components of PM2.5, with a proportion of 46.6%-67.2%. MSW composition had a greater effect on the OC/EC ratios than burning mode. The ratios could be helpful in the analysis of the emission contributions of different MSW components. The proportions of NH4+ and Cl- were the highest in water-soluble ions, accounting for 2.28%-6.35% and 1.04%-14.31%, respectively. Among inorganic elements, Ca, K, Fe, and Ba showed high emission factors. The emission factor of Zn was the highest among heavy metals, and other elements such as Cu, Cr, Sb, and Pb were also enriched. Zn emission was mainly determined by the burning mode; emissions from barrel combustion were approximately 20 times more than that of natural pile-up burning.

Air pollutant emission from the underestimated households' coal consumption source in China.

In order to improve the regional air quality, many control strategies have been developed by Chinese government for reducing air pollutant emission from power plants, industrial and transport sources during the past decade. However, little attention has been paid to residential combustion sources. To fill the knowledge gap, a series of surveys were carried out to investigate the residential energy use in Beijing-Tianjin-Hebei (BTH) region during the period of 2013-2014. Study shows that the actual average amount of residential coal consumption is over 0.7tyr-1 per capita in 2013, which is much higher than that of 0.15tyr-1 per capita reported in the 2014 China Energy Statistical Yearbook (CESY). Combining the investigated activities data with the best available emission factors (EFs), bottom-up method was used to evaluate the potential air pollutant emissions from residential coal combustion in BTH region in 2013. The results indicate that Baoding is the top contributor to the whole BTH region and accounts for approximately 15% of the regional residential emissions in 2013. The spatial pattern of air pollutants shows that high emissions locate in the southeast, along the Yanshan and Taihang Mountains, where much more rural people live and coal combustion is prevalent in winter. The future emission scenario at the end of the 13th Five Year Plan (in 2020) was also predicted based on the policy guidance for the residential coal consumptions in the BTH region. The scenario analysis indicates that air pollutant emissions will drop substantially around 90% because more strict rules will be made for reducing the residential coal consumption. With combined survey information and statistical data, the uncertainty of the emission inventory which was established in this study for the residential sector in the BTH region is reduced and the emission inventory is more reliable for air quality decision making.

Village energy survey reveals missing rural raw coal in northern China: Significance in science and policy.

Burning coal for winter heating has been considered a major contributor to northern China's winter haze, with the district heating boilers holding the balance. However a decade of intensive efforts on district heating boilers brought few improvements to northern China's winter air quality, arousing a speculation that the household heating stoves mainly in rural area rather than the district heating boilers mainly in urban area dominate coal emissions in winter. This implies an extreme underestimation of rural household coal consumption by the China Energy Statistical Yearbooks (CESYs), although direct evidence supporting this speculation is lacking. A village energy survey campaign was launched to gather the firsthand information on household coal consumption in the rural areas of two cities, Baoding (in Hebei province) and Beijing (the capital of China). The survey data show that the rural raw coal consumption in Baoding (5.04 × 103 kt) was approximately 6.5 times the value listed in the official CESY 2013 and exceeded the rural total of whole Hebei Province (4668 kt), revealing a huge amount of raw coal missing from the current statistical system. More importantly, rural emissions of particulate matter (PM) and SO2 from raw coal, which had never been included in widely distributing environmental statistical reports, were found higher than those from industrial and urban household sectors in the two cities in 2013, which highlights the importance of rural coal burning in creating northern China's heavy haze and helps to explain why a number of modeling predictions on ambient pollutant concentrations based on normal emission inventories were more bias-prone in winter season than in other seasons. We therefore recommend placing greater emphasis on the "missing" rural raw coal to help China in its long-term ambition to achieve clean air in the context of rapid economic development.

Increase in polycyclic aromatic hydrocarbon (PAH) emissions due to briquetting: A challenge to the coal briquetting policy.

Both China and UNEP recommend replacing raw coal chunks with coal briquettes in household sector as clean coal technology (CCT), which has been confirmed by the decreased emissions of particulate matter and black carbon. However, the clean effect has never been systematically checked by other pollutants like polycyclic aromatic hydrocarbons (PAHs). In this study, 5 coals with different geological maturities were processed as both chunks and briquettes and burned in 3 typical coal stoves for the measurement of emission factors (EFs) of particle-bound PAHs. It was found that the EFs of 16 parent PAHs, 26 nitrated PAHs, 6 oxygenated PAHs, and 8 alkylated PAHs for coal briquettes were 6.90 ± 7.89, 0.04 ± 0.03, 0.65 ± 0.40, and 72.78 ± 18.23 mg/kg, respectively, which were approximately 3.1, 3.7, 1.9, and 171 times those for coal chunks, respectively. Such significant increases in PAH emissions increased human health risk and challenged the policy of CCT.

Deployment of coal briquettes and improved stoves: possibly an option for both environment and climate.

The use of coal briquettes and improved stoves by Chinese households has been encouraged by the government as a means of reducing air pollution and health impacts. In this study we have shown that these two improvements also relate to climate change. Our experimental measurements indicate that if all coal were burned as briquettes in improved stoves, particulate matter (PM), organic carbon (OC), and black carbon (BC) could be annually reduced by 63 +/- 12%, 61 +/- 10%, and 98 +/- 1.7%, respectively. Also, the ratio of BC to OC (BC/OC) could be reduced by about 97%, from 0.49 to 0.016, which would make the primary emissions of household coal combustion more optically scattering. Therefore, it is suggested that the government consider the possibility of: (i) phasing out direct burning of bituminous raw-coal-chunks in households; (ii) phasing out simple stoves in households; and, (iii) financially supporting the research, production, and popularization of improved stoves and efficient coal briquettes. These actions may have considerable environmental benefits by reducing emissions and mitigating some of the impacts of household coal burning on the climate. International cooperation is required both technologically and financially to accelerate the emission reduction in the world.

Measurements of black and organic carbon emission factors for household coal combustion in China: implication for emission reduction.

Household coal combustion is considered as the greatest emission source for black carbon (BC) and an important source for organic carbon (OC) in China. However, measurements on BC and OC emission factors (EF(BC) and EF(OC)) are still scarce, which result in large uncertainties in emission estimates. In this study, a detailed data set of EF(BC) and EF(OC) for household coal burning was presented on the basis of 38 coal/stove combination experiments. These experiments included 13 coals with a wide coverage of geological maturity which were tested in honeycomb-coal-briquette and raw-coal-chunk forms in three typical coal stoves. Averaged values of EF(BC) are 0.004 and 0.007 g/kg for anthracite in briquette and chunk forms and 0.09 and 3.05 g/kg for bituminous coal, respectively; EF(OC) are 0.06 and 0.10 g/kg for anthracite and 3.74 and 5.50 g/kg for bituminous coal in both forms, respectively. Coal maturity was found to be the most important influencing factor relative to coal's burning forms and the stove's burning efficiency, and when medium-volatile bituminous coals (MVB) are excluded from use, averaged EF(BC) and EF(OC) for bituminous coal decrease by 50% and 30%, respectively. According to these EFs, China's BC and OC emissions from the household sector in 2000 were 94 and 244 gigagrams (Gg), respectively. Compared with previous BC emission estimates for this sector (e.g., 465 Gg by Ohara et al., Atmos. Chem. Phys. 2007, 7, 4419-4444), a dramatic decrease was observed and was mainly attributed to the update of EFs. As suggested by this study, if MVB is prohibited as household fuel together with further promotion of briquettes, BC and OC emissions in this sector will be reduced by 80% and 34%, respectively, and then carbonaceous emissions can be controlled to a large extent in China.

Emission characteristics of carbonaceous particles from various residential coal-stoves in China.

China is thought to be the most important contributor to the global burden of carbonaceous aerosols, and residential coal combustion is the greatest emission source of black carbon (BC). In the present study, two high-efficiency household coal-stoves are tested together with honeycomb-coal-briquettes and raw-coal-chunks of nine different coals. Coal-burning emissions are collected onto quartz fiber filters (QFFs) and analyzed by a thermal-optical transmittance (TOT) method. Emission factors (EFs) of particulate matter (PM), organic carbon (OC), and elemental carbon (EC) are systematically measured, and the average EFs are calculated by taking into account our previous data. For bituminous coal-briquette and -chunk, EFs of PM, OC, and EC are 7.33, 4.16, and 0.08 g/kg and 14.8, 5.93, and 3.81 g/kg, respectively; and for anthracite-briquette and -chunk, they are 1.21, 0.06, and 0.004 g/kg and 1.08, 0.10, and 0.007 g/kg, respectively. Annual estimates for PM, OC, and EC emissions in China are calculated for the years of 2000 and 2005 according to the EFs and coal consumptions, and the results are consistent with our previous estimates. Bituminous coal-chunk contributes 68% and 99% of the total OC and EC emissions from household coal burning, respectively. Additionally, a new model of Aethalometer (AE90) is introduced into the sampling system to monitor the real-time BC concentrations. On one hand, AE90 provides a set of EFs for optical BC in parallel to thermal-optical EC, and these two data are generally comparable, although BC/EC ratios vary in different coal/stove combinations. On the other hand, AE90 offers a chance to observe the variation of BC concentrations during whole burning cycles, which demonstrates that almost all BC emits into the flue during the initial period of 15 min after coal addition into household stoves.