Contribution Of Coal Combustion Research Articles

Variations in the oxidation potential of PM2.5 in an old industrial city in China from 2015 to 2018

PM2.5 pollution in China has decreased dramatically, but how its health effects change is not clear. There are 120 old industrial cities in China, where the sources, composition, and health effects of PM2.5 may be significantly different with other cities. Huangshi, an old industrial city in central China, underwent intense green transformations from 2015 to 2018. In this study, we collected ambient PM2.5 samples in 2015 and 2018 at an urban site in Huangshi. The average PM2.5 concentration decreased from 83.44 ± 48.04 μg/m3 in 2015 to 68.03 ± 39.41 μg/m3 in 2018. However, the average volume-normalized dithiothreitol (DTTv) of PM2.5 increased from 1.38 ± 0.45 nmol/min/m3 to 2.14 ± 1.31 nmol/min/m3 and the DTT normalized by particulate mass (DTTm) increased from 20.6 ± 10.1 pmol/min/μg to 40.07 ± 21.9 pmol/min/μg, indicating increased exposure risk and inherent toxicity. The increased toxicity of PM2.5 might be related to the increased trace elements (TEs) concentrations. The positive matrix factorization and multiple linear regression methods were employed to quantify the contributions of emission sources to PM2.5 and DTTv. The results showed that the contribution of coal combustion, industry, and dust to PM2.5 decreased significantly from 2015 to 2018, while that of vehicle emission and secondary sources increased. Despite the decreased fraction of coal combustion and industry sources, their contribution to DTTv increased slightly, which was caused by the increased intrinsic toxicity. The increased intrinsic toxicity was possibly caused by increased TEs, such as Pb, Cu, and V. Besides, the contribution of vehicle emission to DTTv also increased. Overall, these results provide valuable insights into the effectiveness of controlling strategies in reducing particulate health impacts in old industrial cities, and stress the necessity of formulating toxicity-oriented controlling strategies, with special attention to TEs from coal combustion and industry sources as well as vehicle emissions.

Using sulfur isotopes to constrain the sources of sulfate in PM2.5 during the winter in Jiaozuo City

Sulfate (SO42−) is one of the main driving forces behind the explosive growth of atmospheric fine particulate matter (PM2.5), and it scatters sunlight, contributing to atmospheric cooling. Investigating the sources and transformation of SO42− is crucial for understanding PM2.5 pollution and its implications for climate change. Despite a continuous decline in PM2.5 concentrations in China since 2015, it remains unclear whether there have been changes in the sources and transformation processes of SO42−. Furthermore, previous studies that utilized isotope techniques for source identification have often overlooked the impact of isotope fractionation. This study focuses on atmospheric PM2.5 in Jiaozuo based on samples collected from December 2017 to February 2018. The analysis encompassed both the water-soluble ions and sulfur isotope compositions of SO42− (δ34S–SO42−). By employing a Bayesian isotope mixing model, quantitative analysis of SO42− sources in winter atmospheric PM2.5 in the study area was conducted. The findings revealed that the δ34S–SO42− values of winter PM2.5 ranged from −0.1‰ to 9.8‰, with an arithmetic mean of 4.9 ± 1.5‰ (n = 74). After considering sulfur isotope fractionation effects and the impact of primary SO42−, the calculated results suggested that on average, the contributions of primary SO42−, coal combustion, vehicle exhaust, biomass burning, and oil combustion to the SO42− in winter PM2.5 were 24.9 ± 15.7%, 41.2 ± 2.6%, 27.9 ± 5.3%, 4.8 ± 3.7%, and 1.2 ± 0.7%, respectively. Compared with the clean period, the contribution of the primary SO42− decreased significantly during haze episodes, while the contribution of the secondary SO42− increased. The contribution of coal combustion to the secondary SO42− increased notably by 21.9%, while the contributions from other secondary sulfate remained relatively stable. The lower δ34S values of the atmospheric PM2.5 in Jiaozuo affirm the significant impact of the anthropogenic SO2 input on the sulfur isotope composition of the atmospheric sulfate. Analysis confirmed that the decrease in the contribution of coal combustion to atmospheric SO42− in the study area, indicating the positive effects of regional air pollution control measures. Nevertheless, continued attention should be paid to the influences of coal combustion and vehicle exhaust on regional air pollution.

Long-Term and Seasonal Changes in Emission Sources of Atmospheric Particulate-Bound Pyrene and 1-Nitropyrene in Four Selected Cities in the Western Pacific

Abstract: Estimating the source contribution to polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) in the atmosphere is necessary for developing effective disease control and pollution control measures. The NPAH-PAH combination method (NP method) was used to elucidate the contributions of vehicles and coal/biomass combustion to seasonal and long-term urban atmospheric particulate matter (PM)-bound Pyr and 1-NP concentrations in Kanazawa, Kitakyushu, Shenyang and Shanghai in the Western Pacific region from 1997 to 2021. Among the four cities, Kanazawa demonstrated the lowest Pyr concentration. The contribution of vehicles to Pyr before and after 2010 was 35% and 5%, respectively. The 1-NP concentration was reduced by a factor of more than 1/10. These changes can be attributed to the emission control from vehicles. Kitakyushu revealed the second-lowest Pyr and the lowest 1-NP concentrations. Coal combustion was found to be the main contributor to Pyr, while its contribution to 1-NP increased from 9% to 19%. The large contribution of coal combustion is attributed to iron manufacturers. Shenyang demonstrated the highest atmospheric Pyr concentration with its largest seasonal change. Vehicles are the largest contributors to 1-NP. However, coal combustion, including winter coal heating, contributed 97% or more to Pyr and more than 14% to 1-NP. Shanghai revealed the second-highest Pyr and 1-NP concentrations, but the former was substantially lower than that in Shenyang. Coal combustion was the major contributor, but the contribution of vehicles to Pyr was larger before 2010, which was similar to Kanazawa.

Trace Metals Reveal Significant Contribution of Coal Combustion to Winter Haze Pollution in Northern China

Trace Metals Reveal Significant Contribution of Coal Combustion to Winter Haze Pollution in Northern China

Assessment major NOx sources to nitrate of TSP around the Danjiangkou reservoir using isotopes and a Bayesian isotope mixing model

Nitrate (NO3−) is a key component of atmospheric particulate matter. However, studies quantifying NO3− formation and sources in water source areas remain scarce. This study employs NO3− concentration, dual isotopic analyses (δ15N, δ18O), and SIAR and PSCF models to elucidate NO3− formation mechanisms and apportion sources in the Danjiangkou Reservoir area. The result showed that the concentration of NO3− (0.52 μg m−3-2.39 μg m−3), δ15N–NO3- (−2.3‰-4.2‰) and δ18O–NO3- (64.2‰–96.6‰) values varied seasonally in total suspended particulate matter (TSP). The contribution of the NO2 + ·OH pathway was the highest in summer (84%), while the main contributions came from the N2O5 + H2O and NO3 + VOCs pathways in winter (75%). The SIAR model revealed that the contributions of coal combustion and traffic emissions were 34% and 23%, respectively, indicating that fossil fuel release contributed most. Moreover, the contribution of biomass combustion sources was 31%, and soil emission sources had the least (12%). Considering liquefied petroleum gas, gasoline, and diesel vehicles as traffic emission sources, their contribution to NO3− in TSP increased to 50%. The PSCF analysis indicated that external input areas were predominantly from central Henan Province, northern Hubei Province, and central Shaanxi Province. This study quantitatively analyzed the sources of NO3− in atmospheric particulate matter in water sources for the first time, indicating that controlling the emissions of nitrogen oxides from gasoline cars, heavy-duty diesel trucks, and ships could help alleviate haze pollution and enhance air quality in the Danjiangkou reservoir area.

Increase in Agricultural-Derived NHx and Decrease in Coal Combustion-Derived NOx Result in Atmospheric Particulate N-NH4+ Surpassing N-NO3- in the South China Sea.

The atmospheric deposition of anthropogenic active nitrogen significantly influences marine primary productivity and contributes to eutrophication. The form of nitrogen deposition has been evolving annually, alongside changes in human activities. A disparity arises between observation results and simulation conclusions due to the limited field observation and research in the ocean. To address this gap, our study undertook three field cruises in the South China Sea in 2021, the largest marginal sea of China. The objective was to investigate the latest atmospheric particulate inorganic nitrogen deposition pattern and changes in nitrogen sources, employing nitrogen-stable isotopes of nitrate (δ15N-NO3-) and ammonia (δ15N-NH4+) linked to a mixing model. The findings reveal that the N-NH4+ deposition generally surpasses N-NO3- deposition, attributed to a decline in the level of NOx emission from coal combustion and an upswing in the level of NHx emission from agricultural sources. The disparity in deposition between N-NH4+ and N-NO3- intensifies from the coast to the offshore, establishing N-NH4+ as the primary contributor to oceanic nitrogen deposition, particularly in ocean background regions. Fertilizer (33 ± 21%) and livestock (20 ± 6%) emerge as the primary sources of N-NH4+. While coal combustion continues to be a significant contributor to marine atmospheric N-NO3-, its proportion has diminished to 22 (Northern Coast)-35% (background area) due to effective NOx emission controls by the countries surrounding the South China Sea, especially the Chinese Government. As coal combustion's contribution dwindles, the significance of vessel and marine biogenic emissions grows. The daytime higher atmospheric N-NO3- concentration and lower δ15N-NO3- compared with nighttime further underscore the substantial role of marine biogenic emissions.

Variations of the atmospheric polycyclic aromatic hydrocarbon concentrations, sources, and health risk and the direct medical costs of lung cancer around the Bohai Sea against a background of pollution prevention and control in China

Abstract. The Bohai Sea (BS) region, an area of China that is severely polluted with atmospheric polycyclic aromatic hydrocarbons (PAHs), has received wide attention in recent decades. To characterize the variations of the concentrations and sources of PAHs from June 2014 to May 2019, 15 PAH congeners (Σ15PAHs) were measured in atmospheric samples (N = 228) collected at 12 sites around the BS, and the health risk and direct medical costs associated with lung cancer caused by exposure to PAHs were also estimated. The annual daily average concentration of Σ15PAHs was 56.78 ± 4.75 ng m−3, which was dominated by low molecular weight PAHs (LMW-PAHs) containing three rings (58.7 ± 7.8 %). During the 5-year sampling period, the atmospheric Σ15PAHs concentration reduced by 17.5 % for the whole BS region, with an especially large drop of 51.7 % observed in the tightly controlled area of Tianjin (TJ), which was mainly due to a decrease in the concentration of high molecular weight PAHs (HMW-PAHs) containing five or six rings. Generally, the concentration of Σ15PAHs was highest in winter and lowest in summer, which can mainly be attributed to the change in LMW-PAH concentration. Based on the positive matrix factorization (PMF) model, PAHs in the BS region were mainly ascribed to coal combustion and biomass burning. The PAH contributions of coal combustion and motor vehicles showed different trends for the BS region (PAHs from coal combustion rose by 7.2 % and PAHs from motor vehicles fell by 22.4 %) and for TJ (PAHs from coal combustion fell by 12.6 % and PAHs from motor vehicles rose by 6.9 %). The incidence of lung cancer (ILCR) caused by exposure to atmospheric PAHs decreased by 74.1 % and 91.6 % from 2014 to 2018 in the BS region and in TJ, respectively. This was mainly due to the decrease in the concentration of highly toxic HMW-PAHs and was reflected in USD 10.7 million of savings in direct medical costs of lung cancer caused by exposure to PAHs, which represent a decrease of 46.1 % compared to the corresponding costs before air pollution prevention and control was implemented around the BS. There was an even higher reduction in medical costs of 54.5 % in TJ. Hence, this study proves that implementing pollution prevention and control not only effectively reduced the concentration of pollutants and the risks caused by them, but it also significantly reduced the medical costs of diseases caused by the corresponding exposure.

Quantifying the Nitrogen Sources and Secondary Formation of Ambient HONO with a Stable Isotopic Method.

Nitrous acid (HONO) is a reactive gas that plays an important role in atmospheric chemistry. However, accurately quantifying its direct emissions and secondary formation in the atmosphere as well as attributing it to specific nitrogen sources remains a significant challenge. In this study, we developed a novel method using stable nitrogen and oxygen isotopes (δ15N; δ18O) for apportioning ambient HONO in an urban area in North China. The results show that secondary formation was the dominant HONO formation processes during both day and night, with the NO2 heterogeneous reaction contributing 59.0 ± 14.6% in daytime and 64.4 ± 10.8% at nighttime. A Bayesian simulation demonstrated that the average contributions of coal combustion, biomass burning, vehicle exhaust, and soil emissions to HONO were 22.2 ± 13.1, 26.0 ± 5.7, 28.6 ± 6.7, and 23.2 ± 8.1%, respectively. We propose that the isotopic method presents a promising approach for identifying nitrogen sources and the secondary formation of HONO, which could contribute to mitigating HONO and its adverse effects on air quality.

Linking PAHs concentration, risk to PAHs source shift in soil and water in epikarst spring systems, Southwest China

A systematic assessment of the variations in the ecological risk of PAHs and the key emission sources controlling the variations is of great importance to human health and aquatic organisms. PAH concentrations, composition, source, and ecological risk in soils and water in two different periods (2010–2011 and 2019) of three typical epikarst springs in Southwest China were investigated. Results showed that PAH concentrations in soil and water have an overall downward trend (a reduction of 57 % and 93 %, respectively) in the past 10 years, which is consistent with the downward trend in the relative contribution rate of raw coal production (a 66 % reduction). In terms of composition, the proportion of low-ring PAHs decreased, medium-ring and high-ring PAHs increased in the soil profile. The proportion of low-ring PAHs did not change obviously, the proportion of medium-ring PAHs increased, and the proportion of high-ring PAHs decreased in epikarst springs. The source of PAHs changed remarkably over time, the relative contribution of coal combustion to PAHs decreased from 38 % to 20 %, and the vehicle contribution of PAHs increased from 31 % to 44 % in soils. The relative contribution rate of unburned oil and coke oven and biomass combustion change is less. Furthermore, the ecological risk of PAHs in the soils was reduced from moderate risk 2 to moderate risk 1, the risk in epikarst spring was reduced from high risk to moderate risk 2 after 10 years. This study demonstrates that substituting petroleum and coal with green energies can reduce PAH concentrations and risk.

High-time-resolution chemical composition and source apportionment of PM2.5 in northern Chinese cities: implications for policy

Abstract. Fine particulate matter (PM2.5) pollution is still one of China's most important environmental issues, especially in northern cities during wintertime. In this study, intensive real-time measurement campaigns were conducted in Xi'an, Shijiazhuang, and Beijing to investigate the chemical characteristics and source contributions of PM2.5 and explore the formation of heavy pollution for policy implications. The chemical compositions of PM2.5 in the three cities were all dominated by organic aerosol (OA) and nitrate (NO3-). Results of source apportionment analyzed by a hybrid environmental receptor model (HERM) showed that the secondary formation source contributed more to PM2.5 compared to other primary sources. Biomass burning was the dominant primary source in the three pilot cities. The contribution of coal combustion to PM2.5 is non-negligible in Xi'an and Shijiazhuang but is no longer an important contributor in the capital city of Beijing due to the execution of a strict coal-banning policy. The potential formation mechanisms of secondary aerosol in the three cities were further explored by establishing the correlations between the secondary formation sources and aerosol liquid water content (ALWC) and Ox (O3+NO2), respectively. The results showed that photochemical oxidation and aqueous-phase reaction were two important pathways of secondary aerosol formation. According to source variations, air pollution events that occurred in campaigns were classified into three types: biomass-combustion-dominated, secondary-formation-source-dominated, and a combination of primary and secondary sources. Additionally, this study compares the changes in chemical composition and source contributions of PM2.5 in past decades. The results suggest that the clean-energy replacements for rural households should be urgently encouraged to reduce the primary source emissions in northern China, and collaborative control on ozone and particulate matter needs to be continuously promoted to weaken the atmosphere oxidation capacity for the sake of reducing secondary aerosol formation.

Air pollution prevention in central China: Effects on particulate-bound PAHs from 2010 to 2018

Long-term trends in particulate-bound polycyclic aromatic hydrocarbon (PAH) concentrations in air in Zhengzhou (a severely polluted city in central China) between 2010 and 2018 were studied to assess the effectiveness of an air pollution prevention and control action plan (APPCAP) implemented in 2013. The PM2.5, sum of 16 PAHs (Σ16 PAHs), benzo[a]pyrene (BaP), and BaP toxic equivalent concentrations were high before 2013 but 41%, 77%, 77%, and 78% lower, respectively, after the APPCAP. The maximum daily Σ16 PAHs concentration between 2014 and 2018 was 338 ng/m3, 65% lower than the maximum of 961 ng/m3 between 2010 and 2013. The ratio between the Σ16 PAHs concentrations in winter and summer decreased over time and was 8.0 in 2011 and 1.5 in 2017. The most abundant PAH was benzo[b]fluoranthene, for which the 9-year mean concentration was 14 ± 21 ng/m3 (15% of the Σ16 PAHs concentration). The mean benzo[b]fluoranthene concentration decreased from 28 ± 27 ng/m3 before to 5 ± 4 ng/m3 after the APPCAP (an 83% decrease). The mean daily BaP concentrations were 0.1–62.8 ng/m3, and >56% exceeded the daily standard limit of 2.5 ng/m3 for air. The BaP concentration decreased from 10 ± 8 ng/m3 before to 2 ± 2 ng/m3 after the APPCAP (a 77% decrease). Diagnostic ratios and positive matrix factorization model results indicated that coal combustion and vehicle exhausts were important sources of PAHs throughout the study period, contributing >70% of the Σ16 PAHs concentrations. The APPCAP increased the relative contribution of vehicle exhausts from 29% to 35% but decreased the Σ16 PAHs concentration attributed to vehicle exhausts from 48 to 12 ng/m3. The PAH concentration attributed to vehicle exhausts decreased by 79% even though vehicle numbers strongly increased, indicating that pollution caused by vehicles was controlled well. The relative contribution of coal combustion remained stable but the PAH concentration attributed to coal combustion decreased from 68 ng/m3 before to 13 ng/m3 after the APPCAP. Vehicles made dominant contributions to the incremental lifetime cancer risk (ILCRs) before and after the APPCAP even though the APPCAP decreased the ILCRs by 78%. Coal combustion was the dominant source of PAHs but contributed only 12–15% of the ILCRs. The APPCAP decreased PAH emissions and changed the contributions of different sources of PAHs, and thus strongly affected the overall toxicity of PAHs to humans.

Light absorption properties of brown carbon aerosol after following the switch from coal to natural gas policy in China: A case study of winter particulate matter over Xi'an, northwestern China

To control haze pollution, the Xi'an city in northwestern China replaced coal by natural gas in industrial and household heating at the end of 2017. Following this change we studied here the light absorption properties of brown carbon (BrC)in atmospheric particulate matter (PM2.5) over Xi'an in 2018. PM2.5 samples were collected from November 15 to December 25, 2018, and the light absorption properties of brown carbon in methanol-soluble organic carbon (MSOC) and water-soluble organic carbon (WSOC) were analyzed. Compared to a previous study from the coal combustion period, the mass absorption efficiency (MAE) increased in the sampling period while the radiation-forced absorption fraction of brown carbon relative to elemental carbon reduced, indicating that the light-absorbing capacity and efficiency of brown carbon has improved. Furthermore, highly positive linear relationships (r > 0.80) occur between the absorption coefficient and typical products of biomass burning and vehicle emission, except for coal combustion (r = 0.57). Additionally, an estimation from the positive matrix factorization and multivariable linear regression model results showed that biomass burning, motor vehicle emission, and secondary source took up approximately 89.53% of AbsWSOC,365. The contribution of coal combustion to light absorption BrC was the lowest (7.36% for AbsMSOC,365 and 10.24% for AbsWSOC,365) in our study, which differs from previous studies in Xi'an. Therefore, the emission source of bulk coal combustion has a relatively small influence on the light absorption of BrC in Xi'an.

Identification and contribution of potential sources to atmospheric lead pollution in a typical megacity: Insights from isotope analysis and the Bayesian mixing model

Atmospheric particulate matter (PM) enriched with lead (Pb) has severe irreversible effects on human health. Therefore, identifying the contribution of Pb emission sources is essential for protecting the health of residents. Using the Pb isotopic tracer method, this study explored the seasonal characteristics and primary anthropogenic Pb sources for atmospheric PM in Tianjin in 2019. We calculated the contribution of Pb sources using the end-member and MixSIAR models. The results showed that Pb loaded in PM10 was more abundant in January than in July, and was strongly influenced by meteorological conditions and anthropogenic emissions. The primary Pb sources of the aerosol samples originated from coal combustion and vehicle and steel plant emissions, mainly originating from local Pb emission sources in Tianjin. The PM10-bond Pb in January was influenced by regional transportation and local sources. The MixSIAS model calculated the contribution of coal combustion as approximately 50 %. Compared with that in January, the contribution of coal combustion decreased by 9.6 % in July. Our results indicate that some of the benefits of phased-out leaded gasoline have been short-lived, whereas other industrial activities releasing Pb have increased. Furthermore, the results emphasise the practicability of the Pb isotope tracer source approach for identifying and distinguishing between different anthropogenic Pb inputs. Based on this study, scientific and effective air pollution prevention and control programs can be formulated to provide decision support for the guidance and control of air pollutant emissions.

Winter-autumn air pollution control plan in North China modified the PM2.5 compositions and sources in Central China

The additional impact of emission-reduction measures in North China (NC) during autumn and winter on the air quality of downwind regions is an interesting but less addressed topic. The mass concentrations of routine air pollutants, the chemical compositions, and sources of fine particles (PM2.5) for January 2018, 2019, and 2020 at a megacity of Central China were identified, and meteorology-isolated by a machine-learning technique. Their variations were classified according to air mass direction. An unexpectedly sharp increase in emission-related PM2.5 by 22.7% (18.0 μg m−3) and 25.7% (19.4 μg m−3) for air masses from local and NC in 2019 was observed compared to those of 2018. Organic materials exhibited the highest increase in PM2.5 compositions by 6.90 μg m−3 and 6.23 μg m−3 for the air masses from local and NC. PM2.5 source contributions related to emission showed an upsurge from 1.39 μg m−3 (biomass burning) to 24.9 μg m−3 (secondary inorganic aerosol) in 2019 except for industrial processes, while all reduced in 2020. From 2018 to 2020, the emission-related contribution of coal combustion to PM2.5 increased from 10.0% to 19.0% for air masses from the local area. To support the priority natural gas quotas in northern China, additional coal in cities of southern China was consumed, raising related emissions from transportation activities and road dust in urban regions, as well as additional biofuel consumption in suburban or rural regions. All these activities could explain the increased primary PM2.5 and related precursor NO2. This study gave substantial evidence of air pollution control measures impacting the downwind regions and promote the necessity of air pollution joint control across the administration.

Exploring the Influence of 34S Fractionation From Emission Sources and SO2 Atmospheric Oxidation on Sulfate Source Apportionment Based on Hourly Resolution δ34S‐SO2/SO42−

AbstractSulfate (SO42−) sources are unclear leading to the underestimation of its concentration in the model. Hourly resolution δ34S‐SO2 and δ34S‐SO42− values of three haze episodes (EP1‐EP3) were synchronously collected for the first time to quantify the influence of 34S fractionation from emission sources (e.g., coal combustion) and SO2 atmospheric oxidation on SO2/SO42− source apportionment. After considering the 34S fractionation from coal combustion and atmospheric oxidation, the reasonable and logical source contributions of SO42− were obtained, showing highly consistent with that of Positive Matrix Factorization model results. Considering the 34S fraction from atmospheric oxidation, the source apportionment of SO2/SO42− obtained by hourly resolution δ34S‐SO2 and δ34S‐SO42− can more accurately reflect the dynamic changes of emission sources. Traffic emissions (49%) and coal combustion (46%–65%) were the major contributors to SO2/SO42− in EP1 and EP2‐EP3, respectively. However, obvious deviations of coal combustion contribution were found without considering 34S fractionation from coal combustion. Especially for the northwest transmission channels in EP2‐EP3, the deviation values accounted for 17.1%–38.5% of secondary SO42−. Moreover, δ34S was considered as a more sensitive source indicator than SO2 concentration by the results comparison of 34S technique and air quality model (Nested Air Quality Prediction Model System), which can provide more reliable evidence for SO2 emission control.

Indoor air pollution from the household combustion of coal: Tempo-spatial distribution of gaseous pollutants and semi-quantification of source contribution

Coal is a widely used solid fuel for cooking and heating activities in rural households, whose incomplete combustion in inefficient household stoves releases a range of gaseous pollutants. To evaluate the impact of coal combustion on indoor air quality, this study comprehensively investigated the indoor air pollution of typical gaseous pollutants, including formaldehyde (HCHO), carbon dioxide (CO2), carbon monoxide (CO), total volatile organic compounds (TVOC), and methane (CH4), during coal combustion process in rural households using online monitoring with high tempo-spatial resolution. The indoor concentrations of gaseous pollutants were considerably elevated during the coal combustion period, with the indoor concentrations being significantly higher than those in courtyard air. The levels of several gaseous pollutants (CO2, CO, TVOC, and CH4) in indoor air were much higher during the flaming phase than the de-volatilization and smoldering phases, while HCHO peaked in the de-volatilization phase. The gaseous pollutant concentrations mostly decreased from the room ceiling to the ground level, while their horizontal distribution was relatively uniform within the room. It was estimated that coal combustion accounted for about 71 %, 92 %, 63 %, 59 %, and 21 % of total exposure to indoor CO2, CO, TVOC, CH4, and HCHO, respectively. Improved stove combined with clean fuel could effectively lower the concentrations of CO2, CO, TVOC, and CH4 in indoor air and reduce the contributions of coal combustion to these gaseous pollutants by about 21–68 %. These findings help better understand the indoor air pollution resulting from residential coal combustion and could guide the development of intervention programs to improve indoor air quality in rural households of northern China.

Formation Mechanisms and Source Apportionments of Nitrate Aerosols in a Megacity of Eastern China Based On Multiple Isotope Observations

AbstractInorganic nitrate (NO3−) is a crucial component of fine particulate matter (PM2.5) in haze events in China. Understanding the formation mechanisms of nitrate and the sources of NOx was critical to control the air pollution. In this study, measurements of multiple isotope compositions of nitrate (δ18O‐NO3−, δ17O‐NO3−, and δ15N‐NO3−) in PM2.5 were conducted in Hangzhou from 9 October 2015 to 24 August 2016. Our results showed that oxygen anomaly of nitrate (Δ17O‐NO3−: 20.0‰–37.9‰) and nitrogen isotope of nitrate (δ15N‐NO3−: −2.9‰ to 18.1‰) values were higher in winter and lower in summer. Based on Δ17O‐NO3− observation and a Bayesian model, NO3 radical chemistry was found to dominate the nitrate formation in winter, while photochemical reaction (NO2 + OH) was the main pathway in summer. After considering the nitrogen isotopic fractionation in the NOx(g)‐NO3−(p) conversion, the average contributions of coal combustion, vehicle exhausts, biomass burning, and soil emission were 50% ± 9%, 19% ± 12%, 26% ± 15%, and 5% ± 4%, respectively, to nitrate aerosols during the whole sampling period. Coal combustion was the most important nitrate source in Hangzhou, especially in winter (∼56%). The contribution of soil emission increased significantly in summer due to active soil microbial processes under high temperature environment.

Investigating atmospheric nitrate sources and formation pathways between heating and non-heating seasons in urban North China

In urban North China, nitrate () is a primary contributor to haze formation. So far, the production processes and source apportionments of atmospheric during the heating season (i.e. the wintertime) have not yet been well understood. This study determined δ15N–, δ18O–, and Δ17O– of aerosol samples to compare the potential sources and formation pathways of atmospheric during heating (November to March) and non-heating (April to May) seasons. Combining stable isotope composition with the MixSIAR model based on Δ17O– showed that NO3 + DMS/HC (dimethyl sulfate/hydrocarbon) pathway was the dominant process of atmospheric nitrate formation during the heating season (mean = 52.88 ± 16.11%). During the non-heating season, the contributions of NO3 + DMS/HC (mean = 37.89 ± 13.57%) and N2O5 + H2O (mean = 35.24 ± 3.75%) pathways were comparable. We found that Δ17O– was negatively correlated with wind speed and positively correlated with relative humidity during the heating season, possibly associated with the sources and production of atmospheric . In specific, in a dust storm event, the very low Δ17O– is likely associated with particles from land surface. Under the premise of considering 15N fractionation, the constraint-based on δ15N– illustrated that coal combustion was the major source of NO x emission during the heating season, and the relative contribution of coal combustion decreased rapidly from the heating season (mean = 42.56 ± 15.50%) to the non-heating season (mean = 21.86 ± 4.91%). Conversely, the proportion of NOx emitted by soil microbes rose significantly from the heating (mean = 9.67 ± 5.99%) to non-heating season (mean = 24.02 ± 11.65%). This study revealed differences in the sources and formation processes of atmospheric during the heating and non-heating seasons, which are of significance to atmospheric nitrogen oxide/nitrate pollution mitigation.

Evolution of PM2.5 Chemical Composition and Sources in Nanjing During the Implementation of the APPCAP

To acquire a deeper understanding about the impact of the Air Pollution Prevention and Control Action Plan (APPCAP) on ambient fine particulate matter (PM2.5), measurements of PM2.5 chemical components were conducted in the urban area of Nanjing during the implementation of the APPCAP. Evolution characteristics of several properties of the PM2.5 were studied, including the concentrations, proportions, and enrichment factors of major PM2.5 components and the acidity of the PM2.5. In addition, the source apportion of the PM2.5 was analyzed using the positive matrix factorization (PMF) model. The results showed that during the implementation of the APPCAP, the proportion of sulfate (SO42-) in PM2.5 decreased, whereas the proportions of nitrate (NO-3) and ammonium (NH+4) increased significantly together, from 25.58% in 2014 to 37.15% in 2017. The concentrations of carbon components (OC and EC) decreased in the early stage of the APPCAP; however, the decreasing trend slowed down in the later stage. In particular, the proportion of organic carbon (OC) increased, especially for the secondary organic carbon (SOC). The acidity of the PM2.5 decreased significantly, with the molar equivalent ratio of cations and anions increasing from 0.83 in 2014 to 1.13 in 2017. The contributions of coal combustion and the metallurgical and petrochemical industry to the PM2.5 generally showed a downward trend, whereas the contribution of vehicle emissions increased rapidly, from 8.78% in 2014 to 13.92% in 2017. The contribution of general fugitive dust fluctuated greatly, but that of soil fugitive dust showed an upward trend. This study suggested that the direct PM2.5 emissions, such as those from coal combustion and industries, were effectively controlled during the implementation of the APPCAP; however, the contribution of secondary aerosols became increasingly prominent, which indicates that future policies of PM2.5 pollution control should focus on emission reduction of the precursors such as NOx, NH3, and VOCs. In addition, the effects of increasing alkalization of the PM2.5 and enhanced oxidizability of the atmosphere on the PM2.5 pollution also require further attention.

Vertical Differences of Nitrate Sources in Urban Boundary Layer Based on Tower Measurements

Reducing nitrogen oxide (NOx) emissions is key to limiting fine particulate pollution globally. Nitrogen isotopes are powerful tools for exploring sources of atmospheric nitrate and its precursor NOx. This work performed simultaneous vertical measurements of nitrogen isotopes of nitrate (δ15N(NO3–)) at 8 and 260 m heights on a meteorological tower in Beijing. Although δ15N(NO3–) of the two heights were close, a significant difference (P < 0.01) in the δ15N of nitrogen oxides (NOx) was found in winter after considering the nitrogen isotope fractionation between NOx and the nitrate constrained by the oxygen anomaly (Δ17O) of nitrate. Combining the estimated δ15N of NOx and a Bayesian model, it was found that the proportion of coal combustion to nitrate aerosols was higher at 260 m (54% ± 9%) than that at the ground surface (31% ± 10%) in winter, suggesting that the air masses carrying coal-derived aerosols reached the upper air of Beijing through regional transport. In summer, the vertical variations of nitrate sources were not obvious. Our findings suggest that conventional ground-based observations may underestimate the contribution of coal combustion to atmospheric aerosols in the urban boundary layer as air pollutants are influenced by a combination of local emissions, meteorology, and regional transport.