Life-Course Health Risk Assessment of PM2.5 Elements in China: Exposure Disparities by Species, Source, Age, Gender, and Location.

Key stages in people's lives have particular relevance for their health; the life-course approach stresses the importance of these stages. Here, we applied a life-course approach to analyze the health risks associated with PM2.5-bound elements, which were measured at three sites with varying environmental conditions in eastern China. Road traffic was found to be the primary source of PM2.5-bound elements at all three locations, but coal combustion was identified as the most important factor to induce both cancer risk (CR) and noncancer risk (NCR) across all age groups due to the higher toxicity of elements such as As and Pb associated with coal. Nearly half of NCR and over 90% of CR occurred in childhood (1-6 years) and adulthood (>18 years), respectively, and females have slightly higher NCR and lower CR than males. Rural population is found to be subject to the highest health risks. Synthesizing previous relevant studies and nationwide PM2.5 concentration measurements, we reveal ubiquitous and large urban-rural environmental exposure disparities over China.

Review on magnetic adsorbents for removal of elemental mercury from coal combustion flue gas.

Under the influence of human activities, atmospheric mercury (Hg) concentrations have increased by 450% compared with natural levels. In the context of the Minamata Convention on Mercury, which came into effect in August 2017, it is imperative to strengthen Hg emission controls. Existing Air Pollution Control Devices (APCDs) combined with collaborative control technology can effectively remove Hg2+ and Hgp; however, Hg0 removal is substandard. Compared with the catalytic oxidation method, Hg0 removal through adsorbent injection carries the risk of secondary release and is uneconomical. Magnetic adsorbents exhibit excellent recycling and Hg0 recovery performance and have recently attracted the attention of researchers. This review summarizes the existing magnetic materials for Hg0 adsorption and discusses the removal performances and mechanisms of iron, carbon, mineral-based, and magnetosphere materials. The effects of temperature and different flue gas components, including O2, NO, SO2, H2O, and HCl, on the adsorption performance of Hg0 are also summarized. Finally, different regeneration methods are discussed in detail. Although the research and development of magnetic adsorbents has progressed, significant challenges remain regarding their application. This review provides theoretical guidance for the improvement of existing and development of new magnetic adsorbents.

Environmental Impacts of Coal Combustion Residuals: Current Understanding and Future Perspectives.

On-site solid-waste impoundments, landfills, and receiving water bodies have served as long-term disposal sites for coal combustion residuals (CCRs) across the United States for decades and collectively contain billions of tons of CCR material. CCR components include fine particulate material, minerals, and trace elements such as mercury, arsenic, selenium, lead, etc., which can have deleterious effects on ecosystem functioning and public health. Effects on communities can occur through consumption of drinking water, fish, and other aquatic organisms. The structural failure of impoundments, water infiltration, leakage from impoundments due to poor construction and monitoring, and CCR effluent discharges to water bodies have in the past resulted in harmful environmental impacts. Moreover, the risks posed by CCRs are present to this day, as coal continues to account for 11% of the energy production in the United States. In this Critical Review, the legacy of CCR disposal and the concomitant risks posed to public health and ecosystems are assessed. The resiliency of CCR disposal sites in the context of increased frequency and intensity of storm events and other hazards, such as floods and earthquakes, is also evaluated. We discuss the current state of knowledge on the environmental fate of CCR-derived elements, as well as advances in and limitations of analytical tools, which can improve the current understanding of CCR environmental impacts in order to mitigate the associated risks. An assessment of the 2015 Coal Ash Final Rule is also presented, along with needs to improve monitoring of CCR disposal sites and regulatory enforcement.

Isotopic Signatures and Outputs of Lead from Coal Fly Ash Disposal in China, India, and the United States.

Despite extensive research and technology to reduce the atmospheric emission of Pb from burning coal for power generation, minimal attention has been paid to Pb associated with coal ash disposal in the environment. This study investigates the isotopic signatures and output rates of Pb in fly ash disposal in China, India, and the United States. Pairwise comparison between feed coal and fly ash samples collected from coal-fired power plants from each country shows that the Pb isotope composition of fly ash largely resembles that of feed coal, and its isotopic distinction allows for tracing the release of Pb from coal fly ash into the environment. Between 2000 and 2020, approx. 236, 56, and 46 Gg Pb from fly ash have been disposed in China, India, and the U.S., respectively, posing a significant environmental burden. A Bayesian Pb isotope mixing model shows that during the past 40 to 70 years, coal fly ash has contributed significantly higher Pb (∼26%) than leaded gasoline (∼7%) to Pb accumulation in the sediments of five freshwater lakes in North Carolina, U.S.A. This implies that the release of disposed coal fly ash Pb at local and regional scales can outweigh that of other anthropogenic Pb sources.

Assessment of hazardous radionuclide emission due to fly ash from fossil fuel combustion in industrial activities in India and its impact on public.

Traditionally coal has been extensively used as a dominating fossil fuel in a wide range of industries due to its abundance. In India, industries like thermal power plants, cement industries, iron, and steel industries along with many captive power plants consume a huge quantity of coal each year to meet energy demand. Coal combustion releases blackish-grey colored fly ash waste is one of the most imperative sources of radionuclides like Radium (226Ra), Thorium (232Th), Potassium (40K) and Uranium (238U). The estimated industrial fly ash is ∼308.416 Million Tonnes (MT) in 2019, considered as an emerging environmental problem. This study represents the first-ever radionuclide emission from Indian fly ash generated across various major industries. The results reveal that the estimated 226Ra, 232Th, 238U, and 40K radionuclides were estimated to be ∼27.473 TBq, ∼44.351 TBq, ∼41.089 TBq, and ∼111.091 TBq respectively. The potential radionuclide hotspot regions across the nation are identified, which could be used as an important tool to assess its impact on the chronic exposure of millions of residents living near these sources. Cleaner or green energy could be the best alternative to combat the unseen health disaster. More effective and safe utilization of fly ash can minimize the hazardous effect of radionuclides emission.

Significant coal combustion contribution to water-soluble brown carbon during winter in Xingtai, China: Optical properties and sources.

To understand the characteristics of atmospheric brown carbon (BrC), daily PM2.5 samples in Xingtai, a small city in North China Plain (NCP), during the four seasons of 2018-2019, were collected and analyzed for optical properties and chemical compositions. The light absorption at 365 nm (absλ=365 nm) displayed a strong seasonal variation with the highest value in winter (29.0±14.3 M/m), which was 3.2∼5.4-fold of that in other seasons. A strong correlation of absλ=365 nm with benzo(b)fluoranthene (BbF) was only observed in winter, indicating that coal combustion was the major source for BrC in the season due to the enhanced domestic heating. The mass absorbing efficiency of BrC also exhibited a similar seasonal pattern, and was found to correlate linearly with the aerosol pH, suggesting a positive effect of aerosol acidity on the optical properties and formation of BrC in the city. Positive matrix factorization (PMF) analysis further showed that on a yearly basis the major source for BrC was biomass burning, which accounted for 34% of the total BrC, followed by secondary formation (26.7%), coal combustion (21.3%) and fugitive dust (18%). However, the contribution from coal combustion was remarkably enhanced in winter, accounting for ∼40% of the total. Our work revealed that more efforts of "shifting coal to clean energy" are necessary in rural areas and small cities in NCP in order to further mitigate PM2.5 pollution in China.

A critical review on lead migration, transformation and emission control in Chinese coal-fired power plants.

Coal is widely utilized as an important energy source, but coal-fired power plant was considered to be an important anthropogenic lead emission source. In the present study, the distribution characteristics of lead in coal and combustion by-products are reviewed. Specifically, lead is mainly transferred to ash particles and the formation and migration mechanisms of particulate lead are summarized. Also, targeted measures are proposed to control the formation of fine particulate lead as well as to increase the removal efficiency during the low-temperature flue gas clean process. In detail, interactions between gaseous lead and some coal-bearing minerals or added adsorbents could obviously suppress the formation of fine particulate lead. On the other hand, some efforts (including promoting capture of fine particles, reducing resistivity of particles and strengthening the gas-liquid contact) could be made to improve the fine particulate lead removal capacity. Notably, the formation mechanism of fine particulate lead is still unclear due to the limitations of research methods. Some differences in the removal principles of fine particles and particulate lead make the lead emission precisely control a great challenge. Finally, the environmental potential risk of lead emission from flue gas and ash residues is addressed and further discussed.

Effect of Different Combustion Processes on Atmospheric Nitrous Acid Formation Mechanisms: A Winter Comparative Observation in Urban, Suburban and Rural Areas of the North China Plain.

Atmospheric nitrous acid (HONO) is a dominant precursor of hydroxyl (OH) radicals, and its formation mechanisms are still controversial. Few studies have simultaneously explored effects of different combustion processes on HONO sources. Hereby, synchronous HONO measurement in urban (BJ), suburban (XH) and rural (DBT) areas with different combustion processes is performed in the North China Plain in winter. A box model is utilized to analyze HONO formation mechanisms. HONO concentration is the highest at the DBT site (2.51 ± 1.90 ppb), followed by the XH (2.18 ± 1.95 ppb) and BJ (1.17 ± 1.20 ppb) sites. Vehicle exhaust and coal combustion significantly contribute to nocturnal HONO at urban and rural sites, respectively. During a stagnant pollution period, the NO+OH reaction and combustion emissions are more crucial to HONO in urban and rural areas; meanwhile, the heterogeneous reaction of NO2 is more significant in suburban areas. Moreover, the production rate of OH from HONO photolysis is about 2 orders of magnitude higher than that from ozone photolysis. Consequently, vehicle exhaust and coal combustion can effectively emit HONO, further causing environmental pollution and health risks. It is necessary to expand the implementation of the clean energy transition policy in China, especially in areas with substantial coal combustion.

Coordinatively Unsaturated Selenides over CuFeSe2 toward Highly Efficient Mercury Immobilization.

Metal selenides have been demonstrated as promising Hg0 remediators, while their inadequate adsorption rate primarily impedes their application feasibility. Based on the critical role of coordinatively unsaturated selenide ligands in immobilizing Hg0, this work proposed a novel strategy to enhance the Hg0 adsorption rate of metal selenides by magnitudes by purposefully adjusting the selenide saturation. Copper iron diselenide (CuFeSe2), in which the surface reconstruction tended to occur at ambient temperature, was adopted as the concentrator of unsaturated selenides. The adsorption rate of CuFeSe2 reached as high as 900.71 µg·g-1·min-1, far exceeding those of the previously reported metal selenides by at least 1 magnitude. The excellent resistance of CuFeSe2 to flue gas interference and temperature fluctuation warrants its applicability in real-world conditions. The theoretical investigations and mechanistic interpretations based on density functional theory (DFT) calculation further confirmed the indispensable role of unsaturated selenides in Hg0 adsorption. This work aims not only to develop a Hg0 remediator with extensive applicability in coal combustion flue gas but also to take a step toward the rational design of selenide-based sorbents for diverse environmental remediation by the facile surface functionalization of coordinatively adjustable ligands.

Associations between Source-Specific Fine Particulate Matter and Mortality and Hospital Admissions in Beijing, China.

The health effects of PM2.5 exposure have become a major public concern in developing countries. Identifying major PM2.5 sources and quantifying the health effects at the population level are essential for controlling PM2.5 pollution and formulating targeted emissions reduction policies. In the current study, we have obtained PM2.5 mass data and used positive matrix factorization to identify the major sources of PM2.5. We evaluated the relationship between short-term exposure to PM2.5 sources and mortality or hospital admissions in Beijing, China, using 441 742 deaths and 9 420 305 hospital admissions from 2013 to 2018. We found positive associations for coal combustion and road dust sources with mortality. Increased hospital admission risks were significantly associated with sources of vehicle exhaust, coal combustion, secondary sulfates, and secondary nitrates. Compared to the cool season, excess mortality risk estimates of coal combustion source were significantly higher in the warm season. Our findings show that reducing more toxic sources of PM2.5, especially coal emissions, and developing clean energy alternatives can have critical implications for improving air quality and protecting public health.

Socioeconomic and Demographic Associations with Wintertime Air Pollution Exposures at Household, Community, and District Scales in Rural Beijing, China.

The Chinese government implemented a national household energy transition program that replaced residential coal heating stoves with electricity-powered heat pumps for space heating in northern China. As part of a baseline assessment of the program, this study investigated variability in personal air pollution exposures within villages and between villages and evaluated exposure patterns by sociodemographic factors. We randomly recruited 446 participants in 50 villages in four districts in rural Beijing and measured 24 h personal exposures to fine particulate matter (PM2.5) and black carbon (BC). The geometric mean personal exposure to PM2.5 and BC was 72 and 2.5 µg/m3, respectively. The variability in PM2.5 and BC exposures was greater within villages than between villages. Study participants who used traditional stoves as their dominant source of space heating were exposed to the highest levels of PM2.5 and BC. Wealthier households tended to burn more coal for space heating, whereas less wealthy households used more biomass. PM2.5 and BC exposures were almost uniformly distributed by socioeconomic status. Future work that combines these results with PM2.5 chemical composition analysis will shed light on whether air pollution source contributors (e.g., industrial, traffic, and household solid fuel burning) follow similar distributions.

Anthropogenic Emission Sources of Sulfate Aerosols in Hangzhou, East China: Insights from Isotope Techniques with Consideration of Fractionation Effects between Gas-to-Particle Transformations.

Sulfate (SO42-) is a major species in atmospheric fine particles (PM2.5), inducing haze formation and influencing Earth's climate. In this study, the δ34S values in PM2.5 sulfate (δ34S-SO42-) were measured in Hangzhou, east China, from 2015 September to 2016 October. The result showed that the δ34S-SO42- values varied from 1.6 to 6.4‰ with the higher values in the winter. The estimated fractionation factor (α34Sg→p) from SO2 to SO42- averaged at 3.9 ± 1.6‰. The higher α34Sg→p values in the winter were mainly attributed to the decrease of ambient temperature. We further compared the quantified source apportionments of sulfate by isotope techniques with and without the consideration of fractionation factors. The result revealed that the partitioned emission sources to sulfate with the consideration of the fractionation effects were more logical, highlighting that fractionation effects should be considered in partitioning emission sources to sulfate using sulfur isotope techniques. With considering the fractionation effects, coal burning was the dominant source to sulfate (85.5%), followed by traffic emissions (12.8%) and oil combustion (1.7%). However, the coal combustion for residential heating contributed only 0.9% to sulfate on an annual basis in this megacity.

Toward the Threshold of Radiation Hazards of U in Chinese Coal through the CART Algorithm.

The high volume of coal used for combustion usually leads to a large amount of coal combustion residues (CCRs), which contain the naturally occurring radioactive materials (NORMs) decayed from U and Th in coals. The high radioactivity of NORMs can cause potential harm to humans if the CCRs are used as building materials. The activities of CCRs not only depend on the concentrations of radionuclides but also largely depend on the variations of ash yields of coal. On the other hand, ash yields significantly vary in coal from less than 1-50%. This indicates that similar concentrations of radionuclides in coal with different ash yields generally do not result in similar activities in CCRs. Therefore, it is significant to build a threshold of U in coals with different ash yield levels. In this research, based on the data of 945 coal samples from China and the selected optimal model using the classification and regression tree algorithm, the threshold of U for the radiation hazard is determined to be 7.98 mg/kg for coals with ash yields higher than 20%, while the threshold of U for the radiation hazard is 5.28 mg/kg for coals with ash yields lower than 20%.

Optimization of Iron Removal in the Recovery of Rare-Earth Elements from Coal Fly Ash Using a Recyclable Ionic Liquid.

Rare-earth elements (REEs) are essential for modern technologies, and the United States currently lacks a secure domestic supply. Coal combustion residuals, specifically coal fly ash (CFA), can be a potential source. Our previous work demonstrated that REEs could be preferentially extracted from CFA using the ionic liquid (IL) betainium bis(trifluoromethylsulfonyl)imide ([Hbet][Tf2N]), and the process yielded a mildly acidic REE-rich solution with coextracted Fe and regenerated IL. In this study, we investigated three strategies to limit Fe coextraction: magnetic separation, complexing salts, and ascorbic acid (AA) reduction. Magnetic separation of CFA was ineffective in significantly lowering the Fe content in the IL phase. When NaCl was used instead of NaNO3 during extraction, chloride complexation lowered iron distribution to the IL phase over the aqueous phase (DFe) by five folds, from ∼75 to ∼14, while REE leaching (LREEs) and recovery (RREEs) both increased. Using AA for iron reduction lowered the overall amount of Fe extracted and further decreased DFe to ∼0.16, effectively shifting Fe preference from the IL phase to the aqueous phase. Combining the strategies of NaCl, AA, and supplemental betaine addition, leaching and extraction of REEs from CFA by [Hbet][Tf2N] were achieved in higher efficiency for REE recovery with minimized Fe concentration.

On the fossil and non-fossil fuel sources of carbonaceous aerosol with radiocarbon and AMS-PMF methods during winter hazy days in a rural area of North China plain.

Regional transport is a key source of carbonaceous aerosol in many Chinese megacities including Beijing. The sources of carbonaceous aerosol in urban areas have been studied extensively but are poorly known in upwind rural areas. This work aims to quantify the contributions of fossil and non-fossil fuel emissions to carbonaceous aerosols at a rural site in North China Plain in winter 2016. We integrated online high resolution-time of flight-aerosol mass spectrometer (HR-TOF-AMS) observations and radiocarbon (14C) measurements of fine particles with Positive Matrix Factorization (PMF) analysis as well as Extended Gelencsér (EG) method. We found that fine particle concentration is much higher at the rural site than in Beijing during the campaign (Dec 7, 2016 to Jan 8, 2017). PMF analysis of the AMS data showed that coal-combustion related organic aerosol (CCOA + Oxidized CCOA) and more oxidized oxygenated organic aerosol (MO-OOA) contributed 48% and 30% of organic matter to non-refractory PM1 (NR-PM1) mass. About 2/3 of the OC and EC were from fossil-fuel combustion. The EG method, combining AMS-PMF and 14C data, showed that primary and secondary OC from fossil fuel contribute 35% and 22% to total carbon (TC), coal combustion emission dominates the fossil fuel sources, and biomass burning accounted for 21% of carbonaceous aerosol. In summary, our results confirm that fossil fuel combustion was the dominant source of carbonaceous aerosol during heavy pollution events in the rural areas. Significant emissions of solid fuel carbonaceous aerosols at rural areas can affect air quality in downwind cities such as Beijing and Tianjin, highlighting the benefits of energy transition from solid fuels to cleaner energy in rural areas.

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.

The multiple value characteristics of fly ash from Indian coal thermal power plants: a review.

Coal-powered thermal plants are the primary source of energy production around the globe. More than half (56.89%) of the Indian power plants use coal for power production. Coal burning in power plants results in coal combustion residuals, which contain coal fly ash (CFA) that is recognized as principle by-product. CFA is difficult to characterize due to its broad compositional variation. Hence, the present article summarizes the various physical, chemical, mineralogical, and petrological characterizations of CFA to its use in different applications. Indian coal thermal power plants are found to release two types of CFA: F (fine) and C (coarse). CFA particles are identified as unburned carbon particles with a large fraction of silica oxides, alumina oxides, and iron oxides with a small fraction of calcium oxide (CaO). Morphologically, CFA particles are spherical, with large carbon molecules and a smooth texture surface. In terms of mineralogy; quartz, mullite, magnetite, and hematite are the dominant mineral phases of CFA and tend to be non-plastic, with permeability levels ranging from 8 × 10-6 to 1.87 × 10-4 cms-1. Petrographically, CFA is enriched in inertinite and liptinites as well as collotelinite, collodetrinite, and vitrodetrinite particles. Moreover, CFA is found to be composed of various organic and inorganic particles. By virtue of multiple characterizations, it has been utilized in several applications for decades, which is still quite limited. Therefore, current study aim to provide helpful insights into the potential use of CFA-derived products in different ways to increase sustainability.

Coal Is Dirty, but Where It Is Burned Especially Matters.

Coal abatement actions for pollution reduction often target total coal consumption. The health impacts of coal uses, however, vary extensively among sectors. Here, we modeled the sectorial contributions of coal uses to emissions, outdoor and indoor PM2.5 (particulate matter with an aerodynamic diameter of less than 2.5 mm) concentrations, exposures, and health outcomes in China from 1970 to 2014. We show that in 2014, residential coal accounted for 2.9% of total energy use but 34% of premature deaths associated with PM2.5 exposure, showing that effects were magnified substantially along the causal path. The number of premature deaths attributed to unit coal consumption in the residential sector was 40 times higher than that in the power and industrial sectors. Emissions of primary PM2.5 were more important than secondary aerosol precursors in terms of health consequences, and indoor exposure accounted for 97% and 91% of total premature deaths attributable to PM2.5 from coal combustion in 1974 and 2014, respectively. Our assessment raises a critical challenge in the switching of residential coal uses to effectively mitigate PM2.5 exposure in the Chinese population.

Effect of the Coal Preparation Process on Mercury Flows and Emissions in Coal Combustion Systems.

Coal preparation is effective in controlling primary mercury emissions in coal combustion systems; however, the combustion of coal preparation byproducts may cause secondary emissions. The inconsistent coal preparation statistics, unclear mercury distribution characteristics during coal preparation, and limited information regarding the byproduct utilization pathways lead to great uncertainty in the evaluation of the effect of coal preparation in China. This study elucidated the mercury distribution in coal preparation based on the activity levels of 2886 coal preparation plants, coal mercury content database, tested mercury distribution factors of typical plants, and then traced the mercury flows and emissions in the downstream sectors using a cross-industry mercury flow model. We found that coal preparation altered the mercury flows by reducing 68 tonnes of mercury to sectors such as coking and increasing the flows to byproduct utilization sectors. Combusting cleaned coal rather than raw coal reduced the mercury emissions by 47 tonnes; however, this was offset by secondary mercury emissions. Coal gangue spontaneous combustion and the cement kiln coprocessing process were dominant secondary emitters. Our results highlight the necessity of whole-process emission control of atmospheric mercury based on flow maps. Future comprehensive utilization of wastes in China should fully evaluate the potential secondary mercury emissions.

Evaluation and Integration of Geochemical Indicators for Detecting Trace Levels of Coal Fly Ash in Soils.

Coal combustion residuals (CCRs), in particular, coal fly ash, are one of the major industrial solid wastes in the U.S., and due to their high concentrations of toxic elements, they could pose environmental and human health risks. Yet detecting coal fly ash in the environment is challenging given its small particle size. Here, we explore the utility and sensitivity of using geochemical indicators (trace elements, Ra nuclides, and Pb stable isotopes), combined with physical observation by optical point counting, for detecting the presence of trace levels of coal fly ash particles in surface soils near two coal-fired power plants in North Carolina and Tennessee. Through experimental work, mixing models, and field data, we show that trace elements can serve as a first-order detection tool for fly ash presence in surface soils; however, the accuracy and sensitivity of detection is limited for cases with low fly ash proportion (i.e., <10%) in the soil, which requires the integration of more robust Ra and Pb isotopic tracers. This study revealed the presence of fly ash particles in surface soils from both the recreational and residential areas, which suggests the fugitive emission of fly ash from the nearby coal-fired power plants.