ABSTRACT
In the pursuit of carbon neutrality, China's 2060 targets have been largely anchored in reducing greenhouse gas emissions, with less emphasis on the consequential benefits for air quality and public health. This study pivots to this critical nexus, exploring how China's carbon neutrality aligns with the World Health Organization's air quality guidelines (WHO AQG) regarding fine particulate matter (PM2.5) exposure. Coupling a technology-rich integrated assessment model, an emission-concentration response surface model, and exposure and health assessment, we find that decarbonization reduces sulfur dioxide (SO2), nitrogen oxides (NOx), and PM2.5 emissions by more than 90%; reduces nonmethane volatile organic compounds (NMVOCs) by more than 50%; and simultaneously reduces the disparities across regions. Critically, our analysis reveals that further targeted reductions in air pollutants, notably NH3 and non-energy-related NMVOCs, could bring most Chinese cities into attainment of WHO AQG for PM2.5 5 to 10 years earlier than the pathway focused solely on carbon neutrality. Thus, the integration of air pollution control measures into carbon neutrality strategies will present a significant opportunity for China to attain health and environmental equality.
ABSTRACT
From 2013 to 2019, a series of air pollution control actions significantly reduced PM2.5 pollution in China. Control actions included changes in activity levels, structural adjustment (SA) policy, energy and material saving (EMS) policy, and end-of-pipe (EOP) control in several sources, which have not been systematically studied in previous studies. Here, we integrate an emission inventory, a chemical transport model, a health impact assessment model, and a scenario analysis to quantify the contribution of each control action across a range of major emission sources to the changes in PM2.5 concentrations and associated mortality in China from 2013 to 2019. Assuming equal toxicity of PM2.5 from all the sources, we estimate that PM2.5-related mortality decreased from 2.52 (95 % confidence interval, 2.13-2.88) to 1.94 (1.62-2.24) million deaths. Anthropogenic emission reductions and declining baseline incidence rates significantly contributed to health benefits, but population aging partially offset their impact. Among the major sources, controls on power plants and industrial boilers were responsible for the highest reduction in PM2.5-related mortality (â¼80 %), followed by industrial processes (â¼40 %), residential combustion (â¼40 %), and transportation (â¼30 %). However, considering the potentially higher relative risks of power plant PM2.5, the adverse effects avoided by their control could be â¼2.4 times the current estimation. Our power plant sensitivity analyses indicate that future estimates of source-specific PM2.5 health effects should incorporate variations in individual source PM2.5 effect coefficients when available. As for the control actions, while activity levels increased for most sources, SA policy significantly reduced the emissions in residential combustion and industrial boilers, and EOP control dominated the contribution in health benefits in most sources except residential combustion. Considering the emission reduction potential by source and control actions in 2019, our results suggest that promoting clean energy in residential combustion and enforcing more stringent EOP control in the iron and steel industry should be prioritized in the future.
Subject(s)
Air Pollutants , Air Pollution , Air Pollutants/toxicity , Air Pollutants/analysis , Air Pollution/adverse effects , Air Pollution/analysis , Particulate Matter/adverse effects , Particulate Matter/analysis , Environmental Monitoring/methods , ChinaABSTRACT
The urgent need for decarbonization in China's heating system, comprised of approximately one hundred thousand boilers, is imperative to meet climate and clean air objectives. To formulate national and regional strategies, we developed an integrated model framework that combines a facility-level emission inventory, the Community Multiscale Air Quality (CMAQ) model, and the Global Exposure Mortality Model (GEMM). We then explore the air quality and health benefits of alternative heating decarbonization pathways, including the retirement of coal-fired industrial boilers (CFIBs) for replacement with grid-bound heat supply systems, coal-to-gas conversion, and coal-to-biomass conversion. The gas replacement pathway shows the greatest potential for reducing PM2.5 concentration by 2.8 (2.3-3.4) µg/m3 by 2060, avoiding 23,100 (19,600-26,500) premature deaths. In comparison, the biomass replacement pathway offers slightly lower environmental and health benefits, but is likely to reduce costs by approximately two-thirds. Provincially, optimal pathways vary - Xinjiang, Sichuan, and Chongqing favor coal-to-gas conversion, while Shandong, Henan, Hebei, Inner Mongolia, and Shanxi show promise in CFIBs retirement. Henan leads in environmental and health benefits. Liaoning, Heilongjiang, and Jilin, rich in biomass resources, present opportunities for coal-to-biomass conversion.
Subject(s)
Air Pollutants , Air Pollution , Particulate Matter/analysis , Heating , Air Pollution/prevention & control , Air Pollution/analysis , China , Coal/analysis , Air Pollutants/analysisABSTRACT
Accurately tracking carbon flows is crucial for preventing carbon leakage and allocating responsibility for reducing CO2eq emissions. In this study, we developed an ensemble model to effectively track carbon flows within China's power system. Our approach integrates coal quality tests, individual power plant datasets, a dynamic material-energy flow analysis model, and an extended version of an interconnected power grid model that incorporates transmission and distribution (T&D) losses. Our results not only provide accurate quantification of unit-based CO2eq emissions based on coal quality data but also enable the assessment of emissions attributed to T&D losses and emission shifts resulting from interprovincial coal and electricity trade. Remarkably, for CO2eq emissions from coal-fired units, the disparity between the guideline and our study can be as high as [-95%, 287%]. We identify Guangdong, Hebei, Jiangsu, and Zhejiang provinces as the major importers of both coal and electricity, responsible for transferring nearly half of their user-based emissions to coal and power bases. Significantly, T&D losses, often overlooked, contribute to 15-20% of provincial emissions at the user side. Our findings emphasize the necessity of up-to-date life cycle emissions and spatial carbon shifts in effectively allocating emission reduction responsibilities from the national level to provinces.
Subject(s)
Air Pollutants , Air Pollution , Air Pollutants/analysis , Air Pollution/analysis , Carbon , Power Plants , China , Electricity , Coal/analysis , Carbon Dioxide/analysisABSTRACT
Accurately tracking carbon flows is the first step toward reducing the climate impacts of the iron and steel industry (ISI), which is still lacking in China. In this study, we track carbon flows from coal/mineral mines to end steel users by coupling the cross-process material and energy flow model, point-based emission inventory, and interprovincial trade matrices. In 2020, ISI emitted 2288 Tg of CO2 equivalent (CO2eq, including CH4 and CO2), 96% of which came from energy use and 4% from raw material decomposition. Often overlooked off-gas use and CH4 leakage in coal mines account for 25% of life-cycle emissions. Due to limited scrap resources and a high proportion of pig iron feed, the life-cycle emission intensity of the electric arc furnace (EAF) (1.15 t CO2eq/t steel) is slightly lower than the basic oxygen furnace (BOF) (1.58 t CO2eq/t steel) in China. In addition, over 49% of producer-based emissions are driven by interprovincial coal/coke/steel trade. In particular, nearly all user-based emissions in Zhejiang and Beijing are transferred to steelmaking bases. Therefore, we highlight the need for life-cycle and spatial shifts in user-side carbon management.
Subject(s)
Air Pollutants , Iron , Animals , Swine , Air Pollutants/analysis , Carbon , Steel , Carbon Dioxide/analysis , Coal , ChinaABSTRACT
Small playgrounds situated within residential communities are popular recreational areas. However, heavy metal(loid)s (HMs) in soil or equipment dust may pose a public health risk. This study provides a comprehensive assessment of the health risk associated with HMs exposure at residential playgrounds in cities, a field that has not been thoroughly investigated previously. 70 soil and 70 equipment dust samples were collected from 30 urban and 40 suburban playgrounds in Beijing. Results indicated significant enrichment of Cu, As, and Ni in the soil with Enrichment Factors (EFs) >5 from both anthropogenic and lithogenic sources. Correlation analyses showed that the levels of Be, Cr, Mn, Co, Ni in soil and Be, Mn, As, Cd in dust were positively correlated with the distance to the nearest highway, with p-values < 0.01. Enrichment and correlation analyses contributed to a better understanding of the sources and transport pathways of HMs in urban environment. Based on a site-specific Conceptual Site Model (CSM), the carcinogenic risks (CRs) and Hazard Quotients (HQs) were quantified for residents as the ratio of HMs exposure to reference doses. Risk assessment indicated the mean predicted CR for children and adults exposed to soil was 3.75 × 10-6 and 5.29 × 10-6, respectively, while that at dust exposure scenarios was lower, at 2.47 × 10-6 and 3.49 × 10-6, respectively, all of which were at the upper end of U.S. EPA's acceptable criteria of 1 × 10-6 to 1 × 10-4. Among the HMs, As and Ni were identified as the priority control contaminants due to significant contribution to CRs. Furthermore, the spatial distribution revealed an increasing trend in health risk from the urban center to the suburbs. This study emphasizes the need for effective measures to mitigate potential health risk and enhance the safety of recreational areas, particularly for susceptible individuals.
Subject(s)
Metals, Heavy , Soil Pollutants , Child , Adult , Humans , Beijing , Dust/analysis , Environmental Monitoring/methods , Soil , Soil Pollutants/analysis , Metals, Heavy/analysis , China , Cities , Risk Assessment/methods , Carcinogens/analysisABSTRACT
Boilers involve â¼60% of primary energy consumption in China and emit more air pollutants and CO2 than any other infrastructures. Here, we established a nationwide, facility-level emission data set considering over 185,000 active boilers in China by fusing multiple data sources and jointly using various technical means. The emission uncertainties and spatial allocations were significantly improved. We found that coal-fired power plant boilers were not the most emission-intensive boilers with regard to SO2, NOx, PM, and mercury but emitted the highest CO2. However, biomass- and municipal waste-fired combustion, regarded as zero-carbon technologies, emitted a large fraction of SO2, NOx, and PM. Future biomass or municipal waste mixing in coal-fired power plant boilers can make full use of the advantages of zero-carbon fuel and the pollution control devices of coal-fired power plants. We identified small-size boilers, medium-size boilers using circulating fluidized bed boilers, and large-size boilers located in China's coal mine bases as the main high emitters. Future focuses on high-emitter control can substantially mitigate the emissions of SO2 by 66%, NOx by 49%, PM by 90%, mercury by 51%, and CO2 by 46% at the most. Our study sheds light on other countries wishing to reduce their energy-related emissions and thus the related impacts on humans, ecosystems, and climates.
Subject(s)
Air Pollutants , Air Pollution , Mercury , Humans , Air Pollutants/analysis , Carbon Dioxide , Ecosystem , Coal/analysis , China , Mercury/analysis , Power PlantsABSTRACT
Cytokines play vital roles in the pathogenesis of inflammatory bowel disease. IL17B is protective in the development of colitis. However, how IL17B regulates intestinal inflammation and what cells are regulated by IL17B is still unknown. Here, we aimed to illustrate the IL17B dependent cellular and molecular changes in colon tissue in a mouse colitis model. The results showed that IL17B expression in colon tissues was elevated in inflamed tissues than non-inflamed tissues of IBD patients. Wild type (WT) and Il17b deficient (Il17b -/-) mice were given 2.5% dextran sodium sulfate (DSS) water, and in some case, Il17b -/- mice were treated with recombinant mouse IL17B. IL17B deficiency resulted in severe DSS-induced colitis with exaggerated weight loss, shorter colon length, and elevated proinflammatory cytokines in colon. Reconstitution of Il17b -/- mice with recombinant IL17B alleviated the severity of DSS-induced colitis. Single cell transcriptional analyses of CD45+ immune cells in colonic lamina propria revealed that loss of IL17B resulted in an increased neutrophil infiltration and enhanced inflammatory cytokines in intestinal macrophages in colitis, which were confirmed by real-time PCR and flow cytometry. IL17B treatment also inhibited lipopolysaccharide-induced inflammation in bone marrow-derived macrophages and mice. IL17B inhibits colitis by regulating colonic myeloid cell response. It might represent a novel potential therapeutic approach to treat the colitis.
Subject(s)
Colitis , Interleukin-17 , Animals , Mice , Inflammation , Myeloid Cells/metabolism , Cytokines/metabolism , Immunologic Factors/therapeutic useABSTRACT
Understanding fossil-fuel/food production and consumption patterns is the first step toward reducing the climate impacts of associated methane (CH4) emissions but remains unclear in China. Here, based on the bottom-up method, whole-industrial-chain CH4 emission in China (CH4-CHINA) is developed to track CH4 emissions from production to use and finally to disposal. The estimated Chinese national CH4 emissions in 2020 are 39288.3 Gg (25,230.8-53,345.7 Gg), with 50.4 and 49.6% emissions generated from fossil-fuel and food systems, respectively. â¼130,000 point sources are included to achieve a highly resolved inventory of CH4 emissions, which account for â¼53.5% of the total anthropogenic CH4 emissions in 2020. Our estimate is 36% lower than the Chinese inventory reported to the UNFCCC and 40% lower than EDGAR v6.0, mainly driven by lower emissions from rice cultivation, waste management, and coal supply chain in this study. Based on the emission flow, we observe that previous studies ignored the emissions from natural gas vehicles and residential appliances, coke production, municipal solid waste predisposal, septic tanks, biogas digesters, and food sewage treatment, which totally contribute â¼12.4% of the national anthropogenic CH4 emissions. The results discussed in this study provide critical insights to design and formulate effective CH4 emission mitigation strategies.
Subject(s)
Methane , Waste Management , Methane/analysis , Natural Gas , Coal , ChinaABSTRACT
Interleukin-17 (IL-17) is involved in host defense against bacterial infection. Little is known about the role of IL-17 in A. baumannii-infected pneumonia. Our objective was to investigate the role of IL-17 in pulmonary A. baumannii infection in a mouse model. We infected C57BL/6 mice intra-tracheally (i.t.) with A. baumannii to establish pneumonia model and found A. baumannii infection elevated IL-17 expression in lungs. IL-17-deficient (Il17-/-) mice were resistant to pulmonary A. baumannii infection, showing improved mice survival, reduced bacteria burdens, and alleviated lung inflammation. Further, treatment of A. baumannii-infected Il17-/- mice with IL-17 exacerbated the severity of pneumonia. These data suggest a pathogenic role of IL-17 in pulmonary A. baumannii infection. Further, the infiltration and phagocytic function of neutrophils in broncho-alveolar lavage fluid were detected by flow cytometry. The results showed that Il17-/- mice had increased neutrophil infiltration and enhanced phagocytosis in neutrophils at the early time of infection. Treatment of mice with IL-17 suppressed phagocytic function of neutrophils. All data suggest that IL-17 promotes susceptibility of mice to pulmonary A. baumannii infection by suppressing neutrophil phagocytosis at early time of infection. Targeting IL-17 might be a potential therapeutic strategy in controlling the outcome of A. baumannii pneumonia.
Subject(s)
Acinetobacter Infections , Acinetobacter baumannii , Pneumonia , Animals , Mice , Acinetobacter Infections/microbiology , Acinetobacter Infections/pathology , Disease Models, Animal , Interleukin-17 , Lung/pathology , Mice, Inbred C57BL , Neutrophils/pathology , Pneumonia/pathologyABSTRACT
As the largest emission source in the Pan-Third Pole region, residential solid fuel combustion gains increasing public concern regarding air pollution-associated health impacts. This study firstly developed emission inventories by combining energy statistics, fuel-mix survey, and detailed emission factors considering different fuel types, stove types, and altitudes, and we achieved full regional coverage and increased spatial resolution from 9 × 9 km to 1 km × 1 km. Total CO2, CO, PM2.5, SO2, and NOx emissions (coefficient of variation) were estimated to be 823 Mt (24%), 53 Mt (28%), 4525 kt (48%), 1388 kt (55%), and 1275 kt (46%) in 2020. India, Pakistan, and Bangladesh combined contributed 73, 57, 65, 67, and 69% of total CO2, CO, PM2.5, SO2, and NOx emissions, respectively, due to the large population. The Qinghai-Tibet Plateau had the second-highest emission intensity, mainly due to the high fuel consumption per capita. Unlike the emissions of the Pan-Third Pole in existing Asian inventories, dung cake combustion dominated total PM2.5, SO2, and NOx emissions rather than firewood combustion with proportions of 54, 70, and 67%, respectively. The effect of altitude on combustion efficiencies increased PM2.5 emissions by about 21% from the region. The method and results can provide technical guidance for emission inventory refinement in the Pan-Third Pole and other regions.
Subject(s)
Air Pollutants , Air Pollution , Household Articles , Air Pollutants/analysis , Particulate Matter/analysis , Carbon Dioxide , Air Pollution/analysisABSTRACT
The gaseous or particulate forms of divalent mercury (HgII) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux (FLX). In the new nested-grid GEOS-Chem model, we try to modify the HgII gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg (GOM), particulate-bound Hg (PBM), and PM2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature (T) and organic aerosol (OA) concentrations under different relative humidity (RH). Results showed that with increasing RH, the dominant process of HgII gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgII gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases (NMBs) of monthly gaseous element mercury (GEM), GOM, PBM, WFLX were reduced from -33%-29%, 95%-300%, 64%-261%, 117%-122% to -13%-0%, -20%-80%, -31%-50%, -17%-23%. The improved model explains 69%-98% of the observed atmospheric Hg decrease during 2013-2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.
Subject(s)
Air Pollutants , Mercury , Aerosols , Air Pollutants/analysis , Dust , Environmental Monitoring/methods , Gases , Mercury/analysisABSTRACT
Mercury pollution has attracted worldwide attention due to its toxicity, bioaccumulation and persistence. Cement clinker production is the top emitter of atmospheric mercury in China and the emissions from raw mill systems account for about 85% of all emissions. However, the mercury emission characteristics and mechanisms as a function of time during an operation cycle are still unclear. This study aims to reveal the mercury emission characteristics and mechanisms in cement plants by comprehensively using offline and online field measurements, control experiments and heat transfer analysis. Research results indicated that an intermediate temperature (300-500 °C) desorption and the heterogeneous oxidation of mercury in the precalciner, the selective adsorption of oxidized gaseous mercury (Hg2+) to raw meal, and Hg2+ re-vaporization in the conditioning tower jointly caused an increase in the Hg2+ ratio (15.3%-83.6%) during the mill-off mode. In addition, mercury concentrations remained at approximately 6.5 µg/Nm3 during the mill-on mode while the values reached a peak of 1835.4 µg/Nm3 during the mill-off mode. Thus, atmospheric mercury emissions during the mill-off mode accounted for 35.0%- 71.7% of the emissions during the entire cycle, although the mill-off period only lasted for 5%- 17% of the whole cycle. Our results therefore suggest that supervisory monitoring of mercury in cement clinker production should specify the operating status of raw mills. Mercury control technologies targeting a relatively short period for the mill-off mode can substantially reduce mercury emissions from cement clinker production, and thus, the related impacts on ecosystems and human health.
Subject(s)
Air Pollutants , Mercury , Air Pollutants/analysis , China , Ecosystem , Environmental Monitoring , Environmental Pollution , Humans , Mercury/analysisABSTRACT
Gaseous oxidized mercury (Hg2+) monitoring is one of the largest challenges in the mercury research field, where existing methods cannot simultaneously satisfy the measurement requirements of both accuracy and time precision, especially in high-particulate environments. Here, we verified that dual-stage cation exchange membrane (CEM) sampler is incapable of gaseous elemental mercury (Hg0) uptake even if particulate matter is trapped on CEM, whereas the Hg2+ capture efficiency of the sampler is more than 90%. We then developed a Cation Exchange Membrane-Coupled Speciated Atmospheric Mercury Monitoring System (CSAMS) by coupling the dual-stage CEM sampler with the commercial Tekran 2537/1130/1135 system and configuring a new sampling and analysis procedure, so as to improve the monitoring accuracy of Hg2+ and ensure the simultaneous measurement of Hg0, Hg2+, and Hgp in 2 h time resolution. We deployed the CSAMS in urban Beijing in September 2021 and observed an unprecedented elevated Hg2+ during the daytime with an average amplitude of 510 pg m-3. Using a zero-dimensional box model, the elevated Hg2+ production rate was attributed to high atmospheric oxidant concentrations, Hg0 heterogeneous and interfacial oxidation processes on the surface of atmospheric particles, or potential unknown oxidants.
Subject(s)
Air Pollutants , Mercury , Air Pollutants/analysis , Environmental Monitoring/methods , Gases , Mercury/analysis , Particulate Matter/analysisABSTRACT
The emission of condensable particulate matter (CPM) and its environmental impacts are arousing concern in China with the effective control of filter particulate matter (FPM). This study established an up-to-date and unit-based CPM emission inventory for industrial sectors and systematically evaluated the effects of CPM on primary and secondary PM2.5 in China. In 2020, the national CPM emissions total for industrial sectors was estimated to be 0.98 Tg with uncertainty from -49% to 66%, including 0.62 Tg of organic CPM (CPMorg) and 0.36 Tg of inorganic CPM (CPMin). Totals of 62%, 23% and 8% CPM were emitted from coal-fired power plants, coal-fired industrial boilers and sinter plants, respectively. By filling CPM emissions in PM2.5 simulation, the normalized mean bias (NMB) of model to observation was improved from -27% to -14% in East, North and Central China. The 4 µg/m3 PM2.5 concentration was attributed to CPM emissions in this region, accounting for 10% of observations. On "polluted" days (PM2.5>75 µg/m3), industrial CPM emissions can contribute 7 µg/m3 PM2.5 in North China. Therefore, China should focus on controlling CPM from coal combustion to ensure continuous air quality improvement.
Subject(s)
Air Pollutants , Air Pollution , Air Pollutants/analysis , China , Coal , Environmental Monitoring , Particulate Matter/analysis , Power PlantsABSTRACT
Investigation of mercury (Hg) from atmospheric precipitation is important for evaluating its ecological impacts and developing mitigation strategies. Western China, which includes the Tibetan Plateau and the Xinjiang Uyghur Autonomous Region, is one of the most remote region in the world and is understudied in regards to Hg precipitation. Here we report seesaw-like patterns in spatial variations of precipitation Hg in Western China, based on Hg speciation measurements at nine stations over this remote region. The Hg fraction analyzed included total Hg (HgT), particulate-bound Hg (HgP) and methylmercury (MeHg). Spatially, HgT concentrations and percentage of HgP in precipitation were markedly greater in the westerlies domain than those in the monsoon domain, but the higher wet HgT flux, MeHg concentration and percentage of MeHg in precipitation mainly occurred in the monsoon domain. Similar spatial patterns of wet Hg deposition were also obtained from GEOS-Chem modeling. We show that the disparity of anthropogenic and natural drivers between the two domains are mainly responsible for this seesaw-like spatial patterns of precipitation Hg in Western China. Our study may provide a baseline for assessment of environmental Hg pollution in Western China, and subsequently assist in protecting this remote alpine ecosystem.
Subject(s)
Mercury , Methylmercury Compounds , China , Ecosystem , Environmental Monitoring , Mercury/analysisABSTRACT
In view of the shortcomings of existing artificial neural network (ANN) and support vector regression (SVR) in the application of three-dimensional displacement back analysis, Gaussian process regression (GPR) algorithm is introduced to make up for the shortcomings of existing intelligent inversion methods. In order to improve the generality of the standard GPR algorithm with single kernel function, an improved Gaussian process regression (IGPR) algorithm with combined kernel function is proposed by adding two single kernel functions. In addition, in the training process of IGPR model, the particle swarm optimization (PSO) is combined with the IGPR model (PSO-IGPR) to optimize the parameters of the IGPR model. After the IGPR model can accurately map the relationship between geomechanical parameters and rock mass deformation, the PSO algorithm is directly used to search the best geomechanical parameters to match the deformation calculated by igpr model with the measured deformation of rock mass. The application case of Beikou tunnel shows that the combined kernel function GPR has higher identification accuracy than the single kernel function GPR and SVR model, the IGPR model with automatic correlation determination (ARD) kernel function can obtain higher identification accuracy than the IGPR model with isotropic (ISO) kernel function, and the PSO-IGPR hybrid model based on ARD kernel function has the highest identification accuracy. Therefore, this paper proposes a displacement back analysis method of the PSO-IGPR hybrid algorithm based on ARD kernel function, which can be used to identify the geomechanical parameters of rock mass and solve other engineering problems.
ABSTRACT
Rice grain consumption is a primary pathway of human mercury exposure. To trace the source of rice grain mercury in China, we developed a rice paddy mercury transport and transformation model with a grid resolution of 1 km × 1 km by using the unit cell mass conservation method. The simulated total mercury (THg) and methylmercury (MeHg) concentrations in Chinese rice grain ranged from 0.08 to 243.6 and 0.03 to 238.6 µg/kg, respectively, in 2017. Approximately, 81.3% of the national average rice grain THg concentration was due to atmospheric mercury deposition. However, soil heterogeneity, especially the variation in soil mercury, led to the wide rice grain THg distribution across grids. Approximately, 64.8% of the national average rice grain MeHg concentration was due to soil mercury. In situ methylation was the main pathway via which the rice grain MeHg concentration was increased. The coupled impact of high mercury input and methylation potential led to extremely high rice grain MeHg in partial grids among Guizhou province and junctions with surrounding provinces. The spatial variation in soil organic matter significantly impacted the methylation potential among grids, especially in Northeast China. Based on the high-resolution rice grain THg concentration, we identified 0.72% of grids as heavily polluted THg grids (rice grain THg > 20 µg/kg). These grids mainly corresponded to areas in which the human activities of nonferrous metal smelting, cement clinker production, and mercury and other metal mining were conducted. Thus, we recommended measures that are targeted at the control of heavy pollution of rice grain by THg according to the pollution sources. In addition, we observed a wide spatial variation range of MeHg to THg ratios not only in China but also in other regions of the world, which highlights the potential risk of rice intake.
ABSTRACT
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.
Subject(s)
Air Pollutants , Mercury , Air Pollutants/analysis , China , Coal/analysis , Industry , Mercury/analysis , Physical Phenomena , Power PlantsABSTRACT
Airborne trace elements (TEs) pose a notable threat to human health due to their toxicity and carcinogenicity, whereas their exposures and associated health risks in China remain unclear. Here, we present the first nationwide assessment of spatiotemporal exposure to 11 TEs in China by coupling a bottom-up emission inventory with a modified CMAQ model capable of TE simulation. Associated health risks of 11 TEs are then evaluated using a set of risk assessment models. Our results show that the CMAQ model could reasonably reproduce the spatiotemporal variations of 11 TEs in China compared to observations. We find significant but spatiotemporal-heterogeneous cancer risks associated with high-level exposure of TEs in China. Gridded cell concentrations of hexavalent chromium, arsenic, and nickel in eastern and central China usually exceed China's air quality standard limits, resulting in significant cancer risks that affected over 85% of the entire population in China in 2015. National annual mean population-weighted concentrations of 11 TEs decrease by 9.8-35.6% from 2012 to 2015, largely attributed to emission reduction from coal combustion. Our study provides critical insights for policymakers to implement stricter measures to alleviate health burdens and benefit relevant epidemiological research on airborne TEs.