Present Knowledge and Future Perspectives of Atmospheric Emission Inventories of Toxic Trace Elements: A Critical Review.

Toxic trace elements (TEs) can pose serious risks to ecosystems and human health. However, a comprehensive understanding of atmospheric emission inventories for several concerning TEs has not yet been developed. In this study, we systematically reviewed the status and progress of existing research in developing atmospheric emission inventories of TEs focusing on global, regional, and sectoral scales. Multiple studies have strengthened our understanding of the global emission of TEs, despite attention being mainly focused on Hg and source classification in different studies showing large discrepancies. In contrast to those of developed countries and regions, the officially published emission inventory is still lacking in developing countries, despite the fact that studies on evaluating the emissions of TEs on a national scale or one specific source category have been numerous in recent years. Additionally, emissions of TEs emitted from waste incineration and traffic-related sources have produced growing concern with worldwide rapid urbanization. Although several studies attempt to estimate the emissions of TEs based on PM emissions and its source-specific chemical profiles, the emission factor approach is still the universal method. We call for more extensive and in-depth studies to establish a precise localization national emission inventory of TEs based on adequate field measurements and comprehensive investigation to reduce uncertainty.

Understanding and revealing the intrinsic impacts of the COVID-19 lockdown on air quality and public health in North China using machine learning.

To avoid the spread of COVID-19, China implemented strict prevention and control measures, resulting in dramatic variations in urban and regional air quality. With the complex effect from long-term emission mitigation and meteorology variation, an accurate evaluation of the net effect from lockdown on air quality changes has not been fully quantified. Here, we combined machine learning algorithm and Theil-Sen regression technique to eliminate meteorological and long-term trends effects on air pollutant concentrations and precisely detect concentrations changes those ascribed to lockdown measures in North China. Our results showed that, compared to the same period in 2015-2019, the adverse meteorology during the lockdown period (January 25th to March 15th) in early 2020 increased PM2.5 concentration in North China by 9.8 %, while the reduction of anthropogenic emissions led to a 32.2 % drop. Stagnant meteorological conditions have a more significant impact on the ground-level air quality in the Beijing-Tianjin-Hebei Region than that in Shanxi and Shandong provinces. After further striping out the effect of long-term emission reduction trend, the lockdown-derived NO2, PM2.5, and O3 shown variety change trend, and at -30.8 %, -27.6 %, and +10.0 %, respectively. Air pollutant changes during the lockdown could be overestimated up to 2-fold without accounting for the influences of meteorology and long-term trends. Further, with pollution reduction during the lockdown period, it would avoid 15,807 premature deaths in 40 cities. If with no deteriorate meteorological condition, the total avoided premature should increase by 1146.

Exploring the driving factors of haze events in Beijing during Chinese New Year holidays in 2020 and 2021 under the influence of COVID-19 pandemic.

Unexpected outbreak of the 2019 novel coronavirus (COVID-19) has profoundly altered the way of human life and production activity, which posed visible impacts on PM2.5 and its chemical species. The abruptly emergency reduction in human activities provided an opportunity to explore the synergetic impacts of multi-factors on shaping PM2.5 pollution. Here, we conducted two comprehensive observation measurements of PM2.5 and its chemical species from 1 January to 16 February in Beijing 2020 and the same lunar date in 2021, to investigate temporal variations and reveal the driving factors of haze before and after Chinese New Year (CNY). Results show that mean PM2.5 concentrations during the whole observation were 63.83 and 66.86 µg/m3 in 2020 and 2021, respectively. Higher secondary inorganic species were observed after CNY, and K+, Cl- showed three prominent peaks which associated closely with fireworks burnings from suburb Beijing and surroundings, verifying that they could be used as two representative tracers of fireworks. Further, we explored the impacts of meteorological conditions, regional transportation as well as chemical reactions on PM2.5. We found that unfavorable meteorological conditions accounted for 11.0 % and 16.9 % of PM2.5 during CNY holidays in 2020 and 2021, respectively. Regional transport from southwest and southeast (south) played an important role on PM2.5 during the two observation periods. Higher ratio of NO3-/SO42- were observed under high OX and low RH conditions, suggesting the major pathway of NO3- and SO42- formation could be photochemical process and aqueous-phase reaction. Additionally, nocturnal chemistry facilitated the formation of secondary components of both inorganic and organic. This study promotes understandings of PM2.5 pollution in winter under the influence of COVID-19 pandemic and provides a well reference for haze and PM2.5 control in future.

Heterogeneous Variations on Historical and Future Trends of CO2 and Multiple Air Pollutants from the Cement Production Process in China: Emission Inventory, Spatial-Temporal Characteristics, and Scenario Projections.

Cement production is a major contributor to carbon dioxide (CO2) and multiple hazardous air pollutant (HAP) emissions, threatening climate mitigation and urban/regional air quality improvement. In this study, we established a comprehensive emission inventory by coupling the unit-based bottom-up and mass balance methods, revealing that emissions of most HAPs have been remarkably controlled. However, an increasing 6.0% of atmospheric mercury emissions, as well as 14.1 and 23.7% of fuel-related and process-related CO2 emission growth were witnessed unexpectedly. Industrial adjustment policies have imposed a great impact on the spatiotemporal changes in emission characteristics. Monthly emissions of CO2 and multiple HAPs decreased from December to February due to the "staggered peak production," especially in northern China after implementing the intensified action plan for air pollution control in winter. Upgrading environmental technologies and adjusting capacity structures are identified as dominant driving forces for reducing HAP emissions. Besides, energy intensity improvement can help offset some of the impact caused by the increase in clinker/cement production. Furthermore, scenario analysis results show that ultra-low emission and low-carbon technology transformation constitute the keys to achieve the synergic reduction of CO2 and multiple HAP emissions in the future.

Fine particulate matter (PM2.5/PM1.0) in Beijing, China: Variations and chemical compositions as well as sources.

Particulate matter (i.e., PM1.0 and PM2.5), considered as the key atmospheric pollutants, exerts negative effects on visibility, global climate, and human health by associated chemical compositions. However, our understanding of PM and its chemical compositions in Beijing under the current atmospheric environment is still not complete after witnessing marked alleviation during 2013-2017. Continuous measurements can be crucial for further air quality improvement by better characterizing PM pollution and chemical compositions in Beijing. Here, we conducted simultaneous measurements on PM in Beijing during 2018-2019. Results indicate that annual mean PM1.0 and PM2.5 concentrations were 35.49 ± 18.61 µg/m3 and 66.58 ± 60.17 µg/m3, showing a positive response to emission controls. The contribution of sulfate, nitrate, and ammonium (SNA) played an enhanced role with elevated PM loading and acted as the main contributors to pollution episodes. Discrepancies observed among chemical species between PM1.0 and PM2.5 in spring suggest that sand particles trend to accumulate in the range of 1-2.5 µm. Pollution episodes occurred accompanied with southerly clusters and high formation of SNA by heterogeneous reactions in summer and winter, respectively. Results from positive matrix factorization (PMF) combined with potential source contribution function (PSCF) models showed that potential areas were seasonal dependent, secondary and vehicular sources became much more important compared with previous studies in Beijing. Our study presented a continuous investigation on PM and sources origins in Beijing, which provides a better understanding for further emission control as well as a reference for other cities in developing countries.

Meteorology-normalized variations of air quality during the COVID-19 lockdown in three Chinese megacities.

To avoid the spread of COVID-19, China implemented strict prevention and control measures, resulting in dramatic variations in air quality. Here, we applied a machine learning algorithm (random forest model) to eliminate meteorological effects and characterize the high-resolution variation characteristics of air quality induced by COVID-19 in Beijing, Wuhan, and Urumqi. Our RF model estimates showed that the highest decrease in deweathered PM2.5 in Wuhan (-43.6%) and Beijing (-14.0%) was at traffic stations during lockdown period (February 1- March 15, 2020), while it was at industry stations in Urumqi (-54.2%). Deweathered NO2 decreased significantly in each city (∼30%-50%), whereas accompanied by a notable increase in O3. The diurnal patterns show that the morning peaks of traffic-related NO2 and CO almost disappeared. Additionally, our results suggested that meteorological effects offset some of the reduction in pollutant concentrations. Adverse meteorological conditions played a leading role in the variation in PM2.5 concentration in Beijing, which contributed to +33.5%. The true effect of lockdown reduced the PM2.5 concentrations in Wuhan, Beijing, and Urumqi by approximately 14.6%, 17.0%, and 34.0%, respectively. In summary, lockdown is the most important driver of the decline in pollutant concentrations, but the reduction of SO2 and CO is limited and they are mainly influenced by changing trends. This study provides insights into quantifying variations in air quality due to the lockdown by considering meteorological variability, which varies greatly from city to city, and provides a reference for changes in city scale pollutant concentrations during the lockdown.

A comprehensive emission inventory of hazardous air pollutants from municipal solid waste incineration in China.

The Hazardous air pollutants (HAPs) released from increasing municipal solid waste incineration (MSWI) plants have drawn great concerns in China. However, a full picture of their emission characteristics is still urgently needed, especially after the implementation of stricter emission limits on MSWI. In this study, a comprehensive historical emission inventory of HAPs emitted from MSWI plants in China during the period of 2006-2017 was dedicatedly established by integrating with detailed plant-level activity data and renewed localized emission factors. Overall, HAPs emissions initially increased with years, then peaked or slowed increase in the year 2014, but leveled off after 2016 due to the gradually and fully implementing of newly revised national emission standard (GB18485-2014) applied to mainland China and much stricter local standards for several provinces and cities. It was estimated that totally 50,716 tons (t) of NOx, 13,026 t of CO, 7988 t of SO2, 4399 t of PM, 1943 t of HCl, 9916 kg of Pb, 5901 kg of Mn, 4805 kg of Cu, 3574 kg of Cr, 3329 kg of Ni, 2154 kg of Hg, 1168 kg of Cd, 862 kg of As, 409 kg of Co, 216 kg of Sb, 13 kg of Tl, and 19 g toxic equivalent quantity of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans were emitted from 337 MSWI plants scattered in 30 provinces of mainland China in 2017, respectively. HAPs emissions were heavily concentrated in developed coastal provinces and cities. Scenario analysis highlighted the importance of continuous improvement and upgrade on advanced air pollution control devices and MSWI management to meet the future ultra-low emission limits and minimize the harmful impacts of HAPs on atmospheric environment and public health.

Health impacts and spatiotemporal variations of fine particulate and its typical toxic constituents in five urban agglomerations of China.

Fine particulate matter (PM2.5) and its constituents pose great threatens to public health. The spatial-temporal characteristics of some key chemical constituents, such as sulfate, nitrate, and especially toxic trace elements in China has remained unclear, limiting further studies on evaluating the associated public health. Here, we conduct a two-yearlong (2012 and 2015) air quality simulation by coupling localized emission inventory for primary air pollutants and trace elements with a modified CMAQ model in a domain of China and five urban agglomerations. Associated health burdens of PM2.5 and various toxic trace elements are assessed applying exposure assessment models. The model successfully reproduces air pollution situations. Significant spatial-temporal variations of PM2.5 and chemical constituents are observed, with higher concentrations mainly occurred in North China Plain (NCP), Fenwei Plain (FWP) and Sichuan-Chongqing Basin (SCB). All chemical constituents in PM2.5 show higher concentrations in winter except for sulfate. From 2012 to 2015, the annual averaged PM2.5 concentration and its constituents decreased by 3% -20% nationally and regionally. Smaller reductions of nitrate make PM2.5 pollution become nitrate-dominated, especially in winter. Approximately 0.28 million deaths related to PM2.5 in China are avoided, while the population affected by the cancer risks of Cr (VI) and arsenic has slightly increased from 2012 to 2015. Our findings could provide critical insights on the mitigation of air pollution, as well as benefit for epidemiological studies on air pollutants related health effects.

Field measurements on emission characteristics, chemical profiles, and emission factors of size-segregated PM from cement plants in China.

Cement manufacturing is a major contributor to ambient particulate matter (PM) pollution in China, threatening urban and regional air quality improvement. Here, we tested the typical outlets (kiln tail, kiln head, and coal mill) in one shaft kiln and three rotary kilns to investigate the mass concentrations, size distributions, and chemical compositions of size-segregated PM. Results show that the concentrations of PM in most samples are lower than the strict local emission standards (10 mg/Nm3). We show that the characteristic chemical compositions in PM for most tested outlets are Ca and Ca2+, while for shaft kiln are K, S, K+, and SO42-, and organic carbon. Elemental carbon accounts for a relatively high proportion of PM emitted from coal mills. Meanwhile, unstable and abnormal operating conditions and variations on feed coal compositions will cause high levels of NH4+ and Cl- in PM from the kiln tail/head. Besides, the emission factors (EFs) of PM2.5, PM10, and PM after air pollution control devices for typical outlets of cement plants are calculated, which fall in ranges of 0.16-2.48, 1.49-18.46, and 3.32-35.35 g/(t of clinker), respectively. It suggests that mass emission characteristics, source profiles, and EFs of PM have changed notably as emission standards become more stringent. We believe the newly detailed size-segregated PM EFs and chemical profiles will help update and compile the refined emission inventory for current cement production in China.

Atmospheric Vanadium Emission Inventory from Both Anthropogenic and Natural Sources in China.

Vanadium is a strategically important metal in the world, although sustained exposure under high vanadium levels may lead to notable adverse impact on health. Here, we leverage a bottom-up approach to quantitatively evaluate vanadium emissions from both anthropogenic and natural sources during 1949-2017 in China for the first time. The results show that vanadium emissions increased by 86% from 1949 to 2005 to a historical peak value and then gradually decreased to 12.9 kt in 2017. With the effective implementation of air pollution control measures, vanadium emissions from anthropogenic sources decreased sharply after 2011. During 2011-2017, about half of vanadium emissions came from coal and oil combustion. In addition, industrial processes and natural sources also cannot be ignored, with the total contributions of more than 24%. The high levels of vanadium emissions were mainly distributed throughout the North China Plain and the eastern and coastal regions, especially in several urban agglomerations. Furthermore, the comprehensive evaluation by incorporating contrastive analysis, Monte Carlo approach, and GEOS-Chem simulation shows that vanadium emissions estimated in this study were reasonable and acceptable. The findings of our study provide not only a scientific foundation for investigating the health effects of vanadium but also useful information for formulating mitigation strategies.

Atmospheric emission inventory of hazardous air pollutants from biomass direct-fired power plants in China: Historical trends, spatial variation characteristics, and future perspectives.

The agricultural and forestry biomass direct-fired power generation represents an important technology to promote the low-carbon energy transition and agricultural waste reuse in China. In recent years, emissions of hazardous air pollutants (HAPs) caused by the rapid biomass industrialization have attracted increasing attention. To investigate the characteristics of HAPs emitted from biomass power plants in China, a multiple-year comprehensive emission inventory including NOx, SO2, PM, PM10, PM2.5, and trace elements (As, Cd, Cr, Cu, Hg, Pb, Zn) has been established for the period of 2006-2017. As a result of the emission standard (GB13223-2011), emissions of conventional HAPs have declined since 2014. The results show that national total emissions in 2017 were estimated at 29,516.0 t of NOx, 14,192.1 t of SO2, 4100.7 t of PM, 2353.9 t of PM10, 1630.6 t of PM2.5, 3057.2 kg of As, 1622.8 kg of Cd, 8285.8 kg of Cr, 54,443.4 kg of Cu, 132.9 kg of Hg, 66,325.8 kg of Pb, and 175,587.9 kg of Zn, respectively. The majority of HAPs emissions have been concentrated in eastern, northeastern, and central areas of mainland China. Shandong, Heilongjiang, and Anhui represent the top three provinces with the highest HAPs emissions from 2012 to 2017. Besides, the future emissions in 2025 and 2035 under the ultra-low emission policy are predicted with scenario analysis.

Temporal variation characteristics and source apportionment of metal elements in PM2.5 in urban Beijing during 2018-2019.

To explore high-resolution temporal variation characteristics of atmospheric metal elements concentration and more accurate pollution sources apportionment, online monitoring of metal elements in PM2.5 with 1-h time resolution was conducted in Beijing from August 22, 2018 to August 21, 2019. Concentration of 18 elements varied between detection limit (ranging from 0.1 to 100 ng/m3) and nearly 25 µg/m3. Si, Fe, Ca, K and Al represented major elements and accounted for 93.47% of total concentration during the study period. Compared with previous studies, airborne metal pollution in Beijing has improved significantly which thanks to strict comprehensive control measures under the Clean Air Action Plan since 2013. Almost all elements present higher concentrations on weekdays than weekends, while concentrations of elements associated with dust sources during holidays are higher than those in working days after the morning peak, and there is almost no concentration difference in the evening peak period. Soil and dust, vehicle non-exhaust emissions, biomass, industrial processes and fuel combustion were apportioned as main sources of atmospheric metal pollution, accounting for 63.6%, 18.4%, 16.8%, 1.0% and 0.18%, respectively. Furthermore, main occurrence season of metal pollution is judged by characteristic radar chart of varied metal elements proposed for the first time in this study, for example, fuel combustion type pollution mainly occurs in winter and spring. Results of 72-h backward trajectory analysis of air masses showed that, except for local emissions, atmospheric metal pollution in Beijing is also affected by regional transport from Inner Mongolia, Hebei, the Bohai Sea and Heilongjiang.

Non-Negligible Stack Emissions of Noncriteria Air Pollutants from Coal-Fired Power Plants in China: Condensable Particulate Matter and Sulfur Trioxide.

In this study, we investigated the emission characteristics of condensable particulate matter (CPM) and sulfur trioxide (SO3) simultaneously through ammonia-based/limestone-based wet flue gas desulfurization (WFGD) from four typical coal-fired power plants (CFPPs) by conducting field measurements. Stack emissions of filterable particulate matter (FPM) all meet the Chinese ultralow emission (ULE) standards, whereas CPM concentrations are prominent (even exceed 10 mg/Nm3 from two CFPPs). We find that NH4+ and Cl- increase markedly through the ammonia-based WFGD, and SO42- is generally the main ionic component, both in CPM and FPM. Notably, the occurrence of elemental Se in FPM and CPM is significantly affected by WFGD. Furthermore, the established chemical profiles in FPM and CPM show a distinct discrepancy. In CPM, the elemental S mainly exists as a sulfate, and the metallic elements of Na, K, Mg, and Ca mainly exist as ionic species. Our results may indicate that not all SO3 are included in CPM and they co-exist in stack plume. With the substantial reduction of sulfur dioxide (SO2), S distributed in SO3, CPM, and FPM becomes non-negligible. Finally, the emission factors of CPM and SO3 under typical ULE technical routes fall in the ranges of 74.33-167.83 and 48.76-86.30 g/(t of coal) accordingly.