Health-Oriented Emission Control Strategy of Energy Utilization and Its Co-CO2 Benefits: A Case Study of the Yangtze River Delta, China.

Reducing air pollutants and CO2 emissions from energy utilization is crucial for achieving the dual objectives of clean air and carbon neutrality in China. Thus, an optimized health-oriented strategy is urgently needed. Herein, by coupling a CO2 and air pollutants emission inventory with response surface models for PM2.5-associated mortality, we shed light on the effectiveness of protecting human health and co-CO2 benefit from reducing fuel-related emissions and generate a health-oriented strategy for the Yangtze River Delta (YRD). Results reveal that oil consumption is the primary contributor to fuel-related PM2.5 pollution and premature deaths in the YRD. Significantly, curtailing fuel consumption in transportation is the most effective measure to alleviate the fuel-related PM2.5 health impact, which also has the greatest cobenefits for CO2 emission reduction on a regional scale. Reducing fuel consumption will achieve substantial health improvements especially in eastern YRD, with nonroad vehicle emission reductions being particularly impactful for health protection, while on-road vehicles present the greatest potential for CO2 reductions. Scenario analysis confirms the importance of mitigating oil consumption in the transportation sector in addressing PM2.5 pollution and climate change.

Integrated Benefits of Synergistically Reducing Air Pollutants and Carbon Dioxide in China.

China's advancements in addressing air pollution and reducing CO2 emissions offer valuable lessons for collaborative strategies to achieve diverse environmental objectives. Previous studies have assessed the mutual benefits of climate policies and air pollution control measures on one another, lacking an integrated assessment of the benefits of synergistic control attributed to refined measures. Here, we comprehensively used coupled emission inventory and response models to evaluate the integrated benefits and synergy degrees of various measures in reducing air pollutants and CO2 in China during 2013-2021. Results indicated that the implemented measures yielded integrated benefits value at 6.7 (2.4-12.6) trillion Chinese Yuan. The top five contributors, accounting for 55%, included promoting non-thermal power, implementing end-of-pipe control technologies in power plants and iron and steel industry, replacing residential scattered coal, and saving building energy. Measures demonstrating high synergies and integrated benefits per unit of reduction (e.g., green traffic promotion) yielded low benefits mainly due to their low application, which are expected to gain greater implementation and prioritization in the future. Our findings provide insights into the effectiveness and limitations of strategies aimed at joint control. By ranking these measures based on their benefits and synergy, we offer valuable guidance for policy development in China and other nations with similar needs.

Air Quality, Health, and Equity Benefits of Carbon Neutrality and Clean Air Pathways in China.

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.

Facility-Level Emissions and Synergistic Control of Energy-Related Air Pollutants and Carbon Dioxide in China.

Boilers involve ∼60% 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.

Drivers of High Concentrations of Secondary Organic Aerosols in Northern China during the COVID-19 Lockdowns.

During the COVID-19 lockdown in early 2020, observations in Beijing indicate that secondary organic aerosol (SOA) concentrations increased despite substantial emission reduction, but the reasons are not fully explained. Here, we integrate the two-dimensional volatility basis set into a state-of-the-art chemical transport model, which unprecedentedly reproduces organic aerosol (OA) components resolved by the positive matrix factorization based on aerosol mass spectrometer observations. The model shows that, for Beijing, the emission reduction during the lockdown lowered primary organic aerosol (POA)/SOA concentrations by 50%/18%, while deteriorated meteorological conditions increased them by 30%/119%, resulting in a net decrease in the POA concentration and a net increase in the SOA concentration. Emission reduction and meteorological changes both led to an increased OH concentration, which accounts for their distinct effects on POA and SOA. SOA from anthropogenic volatile organic compounds and organics with lower volatility contributed 28 and 62%, respectively, to the net SOA increase. Different from Beijing, the SOA concentration decreased in southern Hebei during the lockdown because of more favorable meteorology. Our findings confirm the effectiveness of organic emission reductions and meanwhile reveal the challenge in controlling SOA pollution that calls for large organic precursor emission reductions to rival the adverse impact of OH increase.

Sources of Organic Aerosol in China from 2005 to 2019: A Modeling Analysis.

Organic aerosol (OA) is a key component of fine particulate matter (PM2.5) and affects the human health and leads to climate change. With strict control measures for air pollutants during the last decade, the OA concentration in China declined slowly, while its sources remain unclear. In this study, we simulate the primary OA (POA) and secondary OA (SOA) concentrations from 2005 to 2019 with a state-of-the-art air quality model, Community Multiscale Air Quality (CMAQ, version 5.3.2) coupled with a Two-Dimensional Volatility Basis Set (2D-VBS) module, and a long-term emission inventory of full-volatility organic compounds in China and conduct source apportionment and sensitivity analysis. The simulation results show that, from 2005 to 2019, the OA concentration in China decreased from 24.0 to 12.8 µg/m3 with most of the reduction from POA. The OA pollution from residential biomass burning declined 75% from 2005 to 2019, while it is still the major OA source in China. OA pollution from VCP increased by more than 2-fold and became the largest SOA source in China. From 2014 to 2019, the NOx control in China slightly offset the decrease of SOA concentration due to elevated oxidation capacity.

Unpacking the factors contributing to changes in PM2.5-associated mortality in China from 2013 to 2019.

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 (∼80 %), followed by industrial processes (∼40 %), residential combustion (∼40 %), and transportation (∼30 %). However, considering the potentially higher relative risks of power plant PM2.5, the adverse effects avoided by their control could be ∼2.4 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.

Response of organic aerosol in Beijing to emission reductions during the XXIV Olympic Winter Games.

Organic aerosol (OA) serves as a crucial component of fine particulate matter. However, the response of OA to changes in anthropogenic emissions remains unclear due to its complexity. The XXIV Olympic Winter Games (OWG) provided real atmospheric experimental conditions on studying the response of OA to substantial emission reductions in winter. Here, we explored the sources and variations of OA based on the observation of aerosol mass spectrometer (AMS) combined with positive matrix factorization (PMF) analysis in urban Beijing during the 2022 Olympic Winter Games. The influences of meteorological conditions on OA concentrations were corrected by CO and verified by deweathered model. The CO-normalized primary OA (POA) concentrations from traffic, cooking, coal and biomass burning during the OWG decreased by 39.8 %, 23.2 % and 65.0 %, respectively. Measures controlling coal and biomass burning were most effective in reducing POA during the OWG. For the CO-normalized concentration of secondary OA (SOA), aqueous-phase related oxygenated OA decreased by 51.8 % due to the lower relative humidity and emission reduction in precursors, while the less oxidized­oxygenated OA even slightly increased as the enhanced atmospheric oxidation processes may partially offset the efficacy of emission control. Therefore, more targeted reduction of organic precursors shall be enhanced to lower atmospheric oxidation capacity and mitigate SOA pollution.

The development of local ambient air quality standards: A case study of Hainan Province, China.

The ambient air quality standard (AAQS) is a vital policy instrument for protecting the environment and human health. Hainan Province is at the forefront of China's efforts to protect its ecological environment, with an official goal to achieve world-leading air quality by 2035. However, neither the national AAQS nor the World Health Organization guideline offers sufficient guidance for improving air quality in Hainan because Hainan has well met the former while the latter is excessively stringent. Consequently, the establishment of Hainan's local AAQS becomes imperative. Nonetheless, research regarding the development of local AAQS is scarce, especially in comparatively more polluted countries such as China. The relatively high background values and significant interannual fluctuations in air pollutant concentrations in Hainan present challenges in the development of local AAQS. Our research proposes a world-class local AAQS of Hainan Province by reviewing the AAQS in major countries or regions worldwide, analyzing the influence of different statistical forms, and carefully evaluating the attainability of the standard. In the proposed AAQS, the annual mean concentration limit for PM2.5, the annual 95th percentile of daily maximum 8-h mean (MDA8) concentration limit for O3, and the peak season concentration limit for O3 are set at 10, 120, and 85 µg/m3, respectively. Our study indicates that, with effective control policies, Hainan is projected to achieve compliance with the new standard by 2035. The implementation of the local AAQS is estimated to avoid 1,526 (1,253-1,789) and 259 (132-501) premature deaths attributable to long-term exposure to PM2.5 and O3 in Hainan in 2035, respectively.

[Assessing the Environmental and Health Co-benefits of Accelerated Energy Transition and Industrial Restructuring: A Case Study of the BTHS Region].

The Beijing-Tianjin-Hebei-Shandong Region (BTHS Region) is a crucial area for China to achieve synergy between pollution reduction and carbon emissions reduction. The demand for coordinated emissions reduction through source control measures such as energy transition and industrial restructuring are becoming increasingly necessary owing to the limited emissions reductions potential of end-of-pipe control measures. An assessment of the emissions reductions potential through strengthening the end-of-pipe control in the BTHS Region, as well as the environmental and health co-benefits from accelerated energy transition and industrial restructuring, was conducted using scenario simulation analysis based on the REACH model. The results showed that the rapid implementation of the best available end-of-pipe control technologies in the BTHS Region would result in 3.3 µg·m-3 reduction in PM2.5 concentration in 2035, but this would not be sufficient to achieve the PM2.5 concentration control targets. Accelerating the energy transition and the industrial restructuring are necessary for the BTHS Region to achieve air quality standards, which would reduce the PM2.5 concentrations by 6.3 µg·m-3 in 2035. The environmental and health co-benefits brought by the accelerated transition could partially or entirely offset the additional socio-economic cost (compared to that of the current policy efforts) of approximately 0.9%-2.5% of the total regional GDP in achieving the PM2.5 concentration control target paid by the four provinces.

Achieving health-oriented air pollution control requires integrating unequal toxicities of industrial particles.

Protecting human health from fine particulate matter (PM) pollution is the ambitious goal of clean air actions, but current control strategies  largely ignore the role of source-specific PM toxicity. Here, we proposed health-oriented control strategies by integrating the unequal toxic potencies of the most polluting industrial PMs. Iron and steel industry (ISI)-emitted PM2.5 exhibit about one order of magnitude higher toxic potency than those of cement and power industries. Compared with the current mass-based control strategy (prioritizing implementation of ultralow emission standards in the power sector), the proposed health-oriented control strategy (priority control of the ISI sector) could generate 5.4 times higher reduction in population-weighted toxic potency-adjusted PM2.5 exposure among polluting industries in China. Furthermore, the marginal abatement cost per unit of toxic potency-adjusted mass of ISI-emitted PM2.5 is only a quarter of that of the other two sectors under ultralow emission scenarios. We highlight that a health-oriented air pollution control strategy is urgently required to achieve cost-effective reductions in particulate exposure risks.

Improved estimation of rural residential coal emissions considering coal-stove combinations and combustion modes.

Rural residential coal combustion (RRCC) has detrimental effects on air quality, climate, and human health. There are large uncertainties regarding emissions from RRCC owing to the lack of consideration of several key factors (e.g. combination modes of coal and stoves, combustion modes, and high temporal resolution). In this study, we provided a new estimation framework for RRCC emissions through a case study in the Beijing-Tianjin-Hebei (BTH) region, China. The emission estimations were improved according to four aspects, namely (1) coal-specific and stove-specific coal consumption was calculated based on face-to-face field interviews of 6700 valid volunteers/households covering 288 villages in 50 counties; (2) the influences of combustion modes (flaming and smoldering modes) on emissions were considered; (3) emissions of different fuel-stove combinations were estimated based on coal, stove, and combustion mode-specific RRCC consumption and localised emission factors; and (4) a method for emission estimation with high temporal resolution (1 h) was developed. The results indicated that RRCC emitted 413.6 kt SO2, 55.7 kt NOx, 5717.3 kt CO, 149.4 kt VOCs, 167.1 kt PM2.5, 18.2 kt EC, 32.5 kt OC, and 8.2 kt NH3 in 2016. The combination of bituminous coal and an advanced coal stove was the most significant contributor (20.7-71.8%) to various pollutant emissions. Coal combusted under the flaming mode contributed to most (81.9%) of the total coal consumption, and thus emitted the majority (50.8-99.8%) of pollutants, except for VOCs. Meanwhile, that under the smoldering mode only accounted for 18.1% of the total consumption, but contributed 49.2% and 74.7% of the CO and VOCs emissions, respectively. Two clear emission peaks occurred at approximately 7:00-9:00 and 18:00-20:00. The detailed coal consumption and emissions with high temporal and spatial resolution can provide sound data for further research on rural environmental issues and scientific support to pollution control strategies.

Lipin 1 deficiency causes adult-onset myasthenia with motor neuron dysfunction in humans and neuromuscular junction defects in zebrafish.

Lipin 1 is an intracellular protein acting as a phosphatidic acid phosphohydrolase enzyme controlling lipid metabolism. Human recessive mutations in LPIN1 cause recurrent, early-onset myoglobinuria, a condition normally associated with muscle pain and weakness. Whether and how lipin 1 deficiency in humans leads to peripheral neuropathy is yet unclear. Herein, two novel compound heterozygous mutations in LPIN1 with neurological disorders, but no myoglobinuria were identified in an adult-onset syndromic myasthenia family. The present study sought to explore the pathogenic mechanism of LPIN1 in muscular and neural development. Methods: The clinical diagnosis of the proband was compared to the known 48 cases of LPIN1 recessive homozygous mutations. Whole-exome sequencing was carried out on the syndromic myasthenia family to identify the causative gene. The pathogenesis of lipin 1 deficiency during somitogenesis and neurogenesis was investigated using the zebrafish model. Whole-mount in situ hybridization, immunohistochemistry, birefringence analysis, touch-evoke escape response and locomotion assays were performed to observe in vivo the changes in muscles and neurons. The conservatism of the molecular pathways regulated by lipin 1 was evaluated in human primary glioblastoma and mouse myoblast cells by siRNA knockdown, drug treatment, qRT-PCR and Western blotting analysis. Results: The patient exhibited adult-onset myasthenia accompanied by muscle fiber atrophy and nerve demyelination without myoglobinuria. Two novel heterozygous mutations, c.2047A>C (p.I683L) and c.2201G>A (p.R734Q) in LPIN1, were identified in the family and predicted to alter the tertiary structure of LPIN1 protein. Lipin 1 deficiency in zebrafish embryos generated by lpin1 morpholino knockdown or human LPIN1 mutant mRNA injections reproduced the myotomes defects, a reduction both in primary motor neurons and secondary motor neurons projections, morphological changes of post-synaptic clusters of acetylcholine receptors, and myelination defects, which led to reduced touch-evoked response and abnormalities of swimming behaviors. Loss of lipin 1 function in zebrafish and mammalian cells also exhibited altered expression levels of muscle and neuron markers, as well as abnormally enhanced Notch signaling, which was partially rescued by the specific Notch pathway inhibitor DAPT. Conclusions: These findings pointed out that the compound heterozygous mutations in human LPIN1 caused adult-onset syndromic myasthenia with peripheral neuropathy. Moreover, zebrafish could be used to model the neuromuscular phenotypes due to the lipin 1 deficiency, where a novel pathological role of over-activated Notch signaling was discovered and further confirmed in mammalian cell lines.

Trends in ammonia emissions from light-duty gasoline vehicles in China, 1999-2017.

Ammonia (NH3) emitted from motor vehicles is a by-product of measures taken to reduce emissions of other pollutants (e.g. NOx and CO) and has potentially important environmental impacts. NH3 levels can be impacted by various emission standards. However, there is a lack of investigations of the influences from the implementation of different vehicular emission standards on long-term changes in NH3 emissions. To fill this gap, we estimated the inter-annual NH3 emissions of light-duty gasoline vehicles (LDGVs) under different emission standards (State 0 to State V) from 1999 to 2017 and investigated the emission change characteristics under the rapidly developing Chinese economy. Results showed that the NH3 emissions from LDGVs had a sharp, 42-fold increase (from 1.8Gg to 77.9Gg). However, NH3 emissions per capita have begun to decrease with increases in socioeconomic development, presenting an inverted U-shaped tendency as a function of per capita GDP. Further exploration indicated that the decline in emission factors, as determined by upgrades in emission standards, was the decisive factor in promoting the downward trend in per capita emissions. This suggests that continuously upgrading emission standards has offset the increase in NH3 emissions due to the rapid growth of motor vehicles. Quantitative scenario analysis showed a two-stage impact of emission standards on NH3 emissions: emissions would decrease 77% (48%-90% for different years) if State I and State II were not implemented; while if none of standards were upgraded (State III to State V), NH3 emissions would increase 118% (13%-224% for different years), 2-6 times the impacts from the growth of vehicle population and the decline of vehicle kilometres traveled. The data and findings in this study can provide scientific support for understanding air pollution in urban areas and for formulating further vehicle pollution mitigation measures in China and other countries.

Genome-Wide Analysis of Cell-Free DNA Methylation Profiling for the Early Diagnosis of Pancreatic Cancer.

As one of the most malicious cancers, pancreatic cancer is difficult to treat due to the lack of effective early diagnosis. Therefore, it is urgent to find reliable diagnostic and predictive markers for the early detection of pancreatic cancer. In recent years, the detection of circulating cell-free DNA (cfDNA) methylation in plasma has attracted global attention for non-invasive and early cancer diagnosis. Here, we carried out a genome-wide cfDNA methylation profiling study of pancreatic ductal adenocarcinoma (PDAC) patients by methylated DNA immunoprecipitation coupled with high-throughput sequencing (MeDIP-seq). Compared with healthy individuals, 775 differentially methylated regions (DMRs) located in promoter regions were identified in PDAC patients with 761 hypermethylated and 14 hypomethylated regions; meanwhile, 761 DMRs in CpG islands (CGIs) were identified in PDAC patients with 734 hypermethylated and 27 hypomethylated regions (p-value < 0.0001). Then, 143 hypermethylated DMRs were further selected which were located in promoter regions and completely overlapped with CGIs. After performing the least absolute shrinkage and selection operator (LASSO) method, a total of eight markers were found to fairly distinguish PDAC patients from healthy individuals, including TRIM73, FAM150A, EPB41L3, SIX3, MIR663, MAPT, LOC100128977, and LOC100130148. In conclusion, this work identified a set of eight differentially methylated markers that may be potentially applied in non-invasive diagnosis of pancreatic cancer.

Improved estimation of air pollutant emissions from landing and takeoff cycles of civil aircraft in China.

Civil aircraft emissions during landing and takeoff (LTO) are important air pollutant sources, but have been given insufficient attention in China. Accurate estimation of these emissions is limited by a lack of important parameters, such as detailed flight information and the dynamic time in climb and approach modes during LTO that are dependent on mixing layer height (MLH). We developed a flight-time/flight-height relationship using real-time height information in Aircraft Meteorological Data Relay data, and then calculated the actual time for each flight in those two modes based on the actual MLH from meteorological observation. Hourly emissions of civil aircraft were then estimated based on the database of each flight. Total emissions of NOx, CO, SO2, HC and PM from LTO cycles of domestic flights in China during 2015 were 37.78 Gg, 30.25 Gg, 12.00 Gg, 2.38 Gg and 0.75 Gg, respectively. Substantial monthly, daily and hourly variations of emissions due to the flight schedule as well as MLH were calculated. Large differences were found between the new estimation and emissions calculated based on traditional method. Compared with the emissions estimated based on default parameter obtained from International Civil Aviation Organization, the average difference of annual emission among airports with new estimation for various pollutants was approximately 30.3% in climb mode and 81.4% in approach mode; compared with the emissions estimated based on the method proposed by China National Guide, the average difference of annual emission among airports were 37.4% (NOx), 8.4% (CO), 73.1% (HC) and 58.1% (PM) during LTO process. The monthly airport-specific emissions per LTO were also proposed. These can provide necessary and meaningful support for the revision of the values in National Guide.

Chemical composition and sources of PM1 and PM2.5 in Beijing in autumn.

Beijing, the capital of China, suffers from severe atmospheric aerosol pollution; nevertheless, a comprehensive study of the constituents and sources of PM1 is still lacking, and the differences between PM1 and PM2.5 are still unclear. In this study, an intensive observation was conducted to reveal the pollution characteristics of PM1 and PM2.5 in Beijing in autumn. Positive matrix factorization (PMF), backward trajectories and a potential source contribution function (PSCF) model were used to identify the source categories and source areas of PM1 and PM2.5. The results showed that the average concentrations of PM1 and PM2.5 reached 78.20µg/m3 and 95.47µg/m3 during the study period, respectively. PM1 contributed greatly to PM2.5. The PM1/PM2.5 value increased from 73.6% to 90.1% with PM1 concentration growing from <50µg/m3 to >150µg/m3. Higher secondary inorganic aerosol (SIA) proportions (31.3%-70.8%) were found in PM1. The higher fraction of SIA, OC, EC and typical elements in PM1 illustrated that anthropogenic components accumulated more in smaller size particles. Three typical weather patterns causing the heavy pollution in autumn were found as follows: (1) Siberian high and uniform high pressure field, (2) cold front and low-voltage system, and (3) uniform low pressure field. A PMF analysis indicated that secondary aerosols and coal combustion, vehicle, industry, biomass burning, and dust were the important sources of PM, accounting for 53.8%, 8.0%, 13.0%, 13.2% and 12.0% of PM1, respectively, and for 47.5%, 9.9%, 12.4%, 8.4% and 21.8% of PM2.5, respectively. The HYSPLIT and chemical components analysis indicated the potential contribution from biomass burning and fertilization ammonia emissions to PM1 in autumn. The source areas were similar for PM1 and PM1-2.5 under general polluted conditions, but during the heavily polluted periods, the source areas were distributed in farther regions from Beijing for PM1 than for PM1-2.5.

Unregulated pollutant emissions from on-road vehicles in China, 1999-2014.

Multi-year (1999-2014) vehicular unregulated pollutants emissions in China, including SO2, CH4, N2O, NH3, Indeno(1,2,3-cd)pyrene (IPY), Benzo(k)fluoranthene (BkF), Benzo(b)fluoranthene (BbF), Benzo(a)pyrene (BaP), dioxins and furans, were estimated based on emission factors calculated by COPERT. The inter-annual trends, correlation with GDP and population, spatial distribution characteristics, contributions from various vehicle types for the ten pollutants emissions were analyzed. Results showed that the emissions of the above ten pollutants changed from approximately 576.9Gg, 130.0Gg, 8.1Gg, 2.1Gg, 1.0Mg, 1.1Mg, 1.4Mg, 0.5Mg, 7.4g and 15.6g in 1999 to 193.8Gg, 171.1Gg, 79.1Gg, 117.8Gg, 3.5Mg, 6.7Mg, 6.8Mg, 2.9Mg, 37.6g and 79.1g in 2014, respectively. Implementation of stringent sulfur content limit during the past decade reduced approximately 94.4% of the SO2 emission in 2014. CH4 and N2O increased from 1999 to 2011, but began to decrease since 2012; NH3 emission had the highest annual average change rate (35.5%) from 1999 to 2014; PAHs, dioxins and furans increased continuously during the past decade. The vehicular emissions were higher in Guangdong, Shandong, Henan, Jiangsu, Zhejiang and Hebei. Good linear correlation between vehicular emissions and GDP was found (except SO2); in the provinces/municipalities with higher population density, the emission density was also larger, indicating more significant vehicular emissions' potential damage on human health. HDT and PC, PC and MC, PC and BUS were the major contributors to SO2, CH4, N2O emissions, respectively. In 2014, PC was the dominant contributor to NH3 emission; PC, BUS and HDT had higher fraction in the total IPY and BaP emissions; HDT was the major contributor to BkF and BbF emissions. In addition, the uncertainties of estimated emissions were also analyzed based on Monte Carlo simulation.