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Health risks and sources of trace elements and black carbon in PM_(2.5)from 2019 to 2021 in Beijing

Journal of Environmental Sciences 2024年第8期142卷 69-82页

作者： Chenjie Hua Wei Ma Feixue Zheng Yusheng Zhang Jiali Xie Li Ma Boying Song Chao Yan Hongyan Li Zhen Liu Qian Liu Markku Kulmala Yongchun Liu aerosol and haze laboratory Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Institute for Atmospheric and Earth System Research Faculty of ScienceUniversity of HelsinkiHelsinki 00014Finland School of Environment and Safety Taiyuan University of Science and TechnologyTaiyuan 030024China State Key laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

A comprehensive health risk assessment of PM_(2.5)is meaningful to understand the current status and directions regarding further improving air quality from the perspective of human health.In this study,we evaluated the health risks of PM_(2.5)as well as highly toxic inorganic components,including heavy metals(HMs)and black carbon(BC)based on longterm observations in Beijing from 2019 to 2021.Our results showed that the relative risks of chronic obstructive pulmonary disease,lung cancer,acute lower respiratory tract infection,ischemic heart disease,and stroke decreased by 4.07%-9.30%in 2020 and 2.12%-6.70%in2021 compared with 2019.However,they were still at high levels ranging from 1.26 to 1.77,in particular,stroke showed the highest value in 2021.Mn had the highest hazard quotient(HQ,from 2.18 to 2.56)for adults from 2019 to 2021,while Ni,Cr,Pb,As,and BC showed high carcinogenic risks(CR>1.0×10^(-6))for adults.The HQ values of Mn and As and the CR values of Pb and As showed constant or slight upwards trends during our observations,which is in contrast to the downward trends of other HMs and PM_(2.5).Mn,Cr,and BC are crucial toxicants in PM_(2.5).A significant shrink of southern region sourcesof HMs and BCshrank suggests the increased importance of local sources.Industry,dust,and biomass burning are the major contributors to the non-carcinogenic risks,while traffic emissions and industry are the dominant contributors to the carcinogenic risks in Beijing.

关键词： PM_(2.5) Heavy metals Black carbon Health risk Source apportionment

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Sustainable all-weather CO2 utilization by mimicking natural photosynthesis in a single material

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National Science Review 2024年第2期11卷 177-187页

作者： Xianjin Shi Yu Huang Ran Long Zhenyu Wang Liqin Wang Junji Cao Gangqiang Zhu Yujie Xiong State Key laboratory of Loess and Quaternary Geology(SKLLQG) Key Laboratory of Aerosol Chemistry and Physics Institute of Earth EnvironmentChinese Academy of Sciences Center of Excellence in Quaternary Science and Global Change Chinese Academy of Sciences University of Chinese Academy of Sciences Hefei National Research Center for Physical Sciences at the Microscale School of Chemistry and Materials Science and National Synchrotron Radiation Laboratory University of Science and Technology of China Institute of Atmospheric Physics Chinese Academy of Sciences School of Physics and Information Technology Shaanxi Normal University

Solar-driven CO2conversion into hydrocarbon fuels is a sustainable approach to synchronously alleviating the energy crisis and achieving net CO2emissions.However,the dependence of the conversion process on solar illumination hinders its practical application due to the intermittent availability of sunlight at night and on cloudy or rainy days.Here,we report a model material of Pt-loaded hexagonal tungsten trioxide（Pt/h-WO3） for decoupling light and dark reaction processes,demonstrating the sustainable CO2conversion under dark conditions for the first time.In such a material system,hydrogen atoms can be produced by photocatalytic water splitting under solar illumination,stored together with electrons in the h-WO3through the transition of W6+to W5+and spontaneously released to trigger catalytic CO2reduction under dark conditions.Furthermore,we demonstrate using natural light that CH4production can persist at night and on rainy days,proving the accomplishment of all-weather CO2conversion via a sustainable way.

关键词： sustainable CO2 utilization artificial photosynthesis all-weather application charge storage

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Impact of Atmospheric Transmittance and NLTE Correction on Simulation of High Spectral Infrared Atmospheric Sounder onboard FY-3E

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Journal of Meteorological Research 2024年第2期38卷 225-234页

作者： Chenggege FANG Peiming DONG Yang HAN Wanlin KAN Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters Key Laboratory for Aerosol-Cloud-Precipitation of China Meteorological AdministrationNanjing University of Information Science&TechnologyNanjing 210044 Donghai laboratory Zhoushan 316021 State Key laboratory of Severe Weather Chinese Academy of Meteorological SciencesChina Meteorological AdministrationBeijing 100081 CMA Earth System Modeling and Prediction Centre China Meteorological Administration(CMA)Beijing 100081 Key laboratory of Transportation Meteorology of China Meteorological Administration Nanjing Joint Institute for Atmospheric SciencesNanjing 210041

With the launch of the first civilian early-morning orbit satellite Fengyun-3E(FY-3E),higher demands are placed on the accuracy of radiative transfer simulations for hyperspectral infrared data.Therefore,several key issues are investigated in the paper.First,the accuracy of the fast atmospheric transmittance model implemented in the Advanced Research and Modeling System(ARMS)has been evaluated with both the line-by-line radiative transfer model(LBLRTM)and the actual satellite observations.The results indicate that the biases are generally less than 0.25 K when compared to the LBLRTM,while below 1.0 K for the majority of the channels when compared to the observations.However,during both comparisons,significant biases are observed in certain channels.The accuracy of Hyperspectral Infrared Atmospheric Sounder-II(HIRAS-II)onboard FY-3E is comparable to,and even superior to that of the Cross-track Infrared Sounder(CrIS)onboard NOAA-20.Furthermore,apodization is a crucial step in the processing of hyperspectral data in that the apodization function is utilized as the instrument channel spectral response function to produce the satellite channel-averaged transmittance.To further explore the difference between the apodized and unapodized simulations,Sinc function is adopted in the fast transmittance model.It is found that the use of Sinc function can make the simulations fit the original satellite observations better.When simulating with apodized observations,the use of Sinc function exhibits larger deviations compared to the Hamming function.Moreover,a correction module is applied to minimize the impact of Non-Local Thermodynamic Equilibrium(NLTE)in the shortwave infrared band.It is verified that the implementation of the NLTE correction model leads to a significant reduction in the bias between the simulation and observation for this band.

关键词： high spectral infrared sounding atmospheric transmittance apodization Non-Local Thermodynamic Equilibrium Fengyun-3E(FY-3E)

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Molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain,Northwest China:The importance of biomass burning

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Particuology 2024年第6期89卷 44-56页

作者： Yali Liu Minxia Shen Haijiao Liu Wenting Dai Weining Qi Yifan Zhang Lu Li Yue Cao Xin Wang Xiao Guo Yingkun Jiang Jianjun Li State Key laboratory of Loess and Quaternary Geology Key Lab of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi'an 710061China Xi'an Institute for Innovative Earth Environment Research Xi'an 710061China National Observation and Research Station of Regional Ecological Environment Change and Comprehensive Management in the Guanzhong Plain ShaanxiChina

The concentration of PM_(2.5)has considerably reduced in recent years,but remains relatively high in China.In particular,the increasing contribution of organic compounds to PM_(2.5)generates popular pressure for further reductions,resulting in an urgent need to study organic aerosol(OA).To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain,Northwest China,PM_(2.5)samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer compounds.The mean concentration of total measured organic compounds is 662±296 ng/m^(3)in summer and 3258±1925 ng/m^(3)in winter.Levoglucosan is the most abundant single compound found throughout the sampling period,which is a crucial tracer for biomass burning emissions,preliminary suggesting that biomass burning is an essential source of OA.In summer,organic compounds such as lipid compounds,sugar compounds,and polycyclic aromatic hydrocarbons(PAHs),more come from higher plants,wood burning,vehicle exhausts,plastic waste,and other direct emission sources.Oxygenated PAHs(OPAHs),nitrophenols,and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors,especially photochemical oxidation.However,in winter,most of the increases in concentrations of organic compounds are attributed to biomass burning.The analysis of a haze event(14–19 January 2017)during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity(49.1%±13.5%).The main reason for the growth of OA in this haze event is the accumulation of primary OA(POA).The source apportionment by the positive matrix factorization(PMF)model shows that biomass burning(37.1%)is the primary source of OA in the rural regions of the Guanzhong Plain,especially in winter(40.6%).The contribution of secondary formation decreases from 26.0%in summer to 16.9%in winter,and the contribution of fossil

关键词： Organic aerosol Molecular composition Seasonal variation Source apportionment Guanzhong Plain

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Characteristics of bioaerosols under high-ozone periods,haze episodes,dust storms,and normal days in Xi'an,China

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Particuology 2024年第7期90卷 140-148页

作者： Yiming Yang Liu Yang Xiaoyan Hu Zhenxing Shen Department of Environmental Science and Engineering Xi’an Jiaotong UniversityXi’an710049China Key Lab of aerosol Chemistry&Physics SKLLQGInstitute of Earth EnvironmentChinese Academy of SciencesXi’an710049China

The characteristics of bioaerosols and their effects on human beings'health have become a major public concern in the recent years.This study compared the characteristics of bioaerosols under different types of pollution(high-ozone[HO]episodes,haze episodes,and dust storms[DSs]),with those of bioaerosols on normal days(NDs)in Xi'an,China.The concentrations,diurnal variations,and size distribution of bacteria,fungi,and total airborne microbes(TAMs)were investigated.The results showed that the bacterial and fungal concentrations were the highest during DSs and on NDs,reaching 425.2 and 956.9 colony-forming units/m^(3),respectively.The concentration of TAMs was the highest during HO episodes,reaching 10.7×10^(6)cells/m^(3),which was significantly higher than that during the other events.The maximum concentrations of bacteria and fungi during HO episodes were observed in the morning,while they appeared separately in the morning and evening during haze episodes.Bacteria and TAMs during DSs reached peak concentrations in the morning and evening,which is opposite to the particulate matter(PM)distribution pattern.On NDs,temperature and relative humidity had significant effects on bioaerosols.The size distributions of airborne bacteria exhibited bimodal patterns,whereas unimodal distributions were observed for fungi.Fungi mainly attached in fine particles(haze episodes and DSs,respectively,which means that fungi were easily penetrated into the human respiratory system.The evaluation of influence factors revealed that PM_(2.5) and PM10 had negative effects on fungal concentration during DSs,and ozone concentration and temperature were inversely correlated with fungal concentration during HO episodes.These results provide valuable reference data for elucidating the formation and evolution of bioaerosols under different types of pollution.

关键词： Bacteria Fungi Total airborne microbe Different air pollution types Influence factors

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Recent progress of MgO-based materials in CO_(2) adsorption and conversion:Modification methods,reaction condition,and CO_(2) hydrogenation

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Chinese Chemical Letters 2024年第5期35卷 57-65页

作者： Zixuan Zhu Xianjin Shi Yongfang Rao Yu Huang Key laboratory of aerosol Chemistry&Physics State Key Laboratory of Loess and Quaternary Geology(SKLLQG)Institute of Earth EnvironmentChinese Academy of Sciences(CAS)Xi’an 710061China Center for Excellence in Quaternary Science and Global Change Chinese Academy of SciencesXi’an 710061China University of Chinese Academy of Sciences Beijing 100049China Department of Environmental Science and Engineering Xi’an Jiaotong UniversityXi’an 710049China

Integrated CO_(2) capture and conversion of(ICCC)is one of the most effective solutions to reduce anthropogenic CO_(2) emissions,which has attracted extensive public attention.Dual functional materials(DFMs),including adsorbent and catalyst,are the key components to achieve ICCC.Magnesium oxide(MgO)is an ideal adsorbent for ICCC,since it is characterized by high theoretical adsorption capacity,low cost,low energy consumption and extensive sources.It can also be used as DFMs in combination with the Ni catalysts.MgO not only can act as an adsorbent in DFMs but also enhance the catalytic performance of Ni.This review summarizes the advantages and modification methods of MgO as adsorbent and the influence of its adsorption conditions on the adsorption performance.Moreover,the important role of MgO in facilitating the catalytic conversion of CO_(2) is highlighted.Future research focuses are proposed for the development of MgO based DFMs with high adsorption capacity,high stability,conversion,and selectivity as well as low cost and energy consumption.

关键词： CO_(2) ICCC MgO Adsorption Conversion

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Enhancement and Removal of PM2.5 by Cold and Warm Air Masses Accompanying Certain Synoptic Weather Systems across Hangzhou, China during 2014–2020

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Journal of Meteorological Research 2024年第3期38卷 620-634页

作者： Bu YU Feng CHEN Hanqing KANG Bin ZHU Hongnian LIU Hangzhou Meteorological Bureau Hangzhou International Urbanology Research Center for Urban Governance Studies Zhejiang Institute of Meteorological Sciences Key laboratory for aerosol–Cloud–Precipitation of China Meteorological Administration Nanjing University of Information Science&Technology School of Atmospheric Sciences Nanjing University

Local air pollution is strongly affected by synoptic weather systems,such as fronts,troughs,low-altitude vortices,or high-altitude ridges.Nevertheless,few studies have analyzed the meteorological properties of cold or warm air masses associated to these systems and their impact on local air quality.In this study,hourly observations of fine particulate matter (diameter of up to 2.5μm,i.e.,PM2.5),wind （V）,temperature （T）,pressure （P）,and precipitation （R）,acquired in Hangzhou in 2014–2020,were analyzed.From this analysis,weather patterns were categorized into 27types;89 and 94 cases illustrating the passage of warm and cold air masses over Hangzhou were identified,respectively;the influence of air mass temperature,wind speed,and wind direction on PM2.5concentrations and local accumulation or removal was quantified.The main results are as follows.（1） Pollution events occurred more frequently for cold than for warm air masses,but average pollutant concentration was lower for cold air masses;（2） 48%of the cold air mass cases corresponded to PM2.5decreases and 52%to PM2.5increases,with strong cold air masses(?T24h>4℃;|V|average>4 m s-1) markedly reducing local pollution,but weak cold air masses (?T24h4℃) reduced the PM2.5concentration whereas weaker winds (|V|average<2 m s-1) increased it;and （4） PM2.5concentration decreased sharply within 4 h after the passage of strong cold air masses,but more gradually within 14 h after the passage of strong warm air masses.These results considerably improve the current understanding of the influence of cold and warm air masses on local pollution patterns.

关键词： weather type air mass enhancement removal meteorological condition

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Improvement of cloud microphysical parameterization and its advantages in simulating precipitation along the Sichuan-Xizang Railway

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Science China Earth Sciences 2024年第3期67卷 856-873页

作者： Xiaoqi XU Zhiwei HENG Yueqing LI Shunjiu WANG Jian LI Yuan WANG Jinghua CHEN Peiwen ZHANG Chunsong LU China Meteorological Administration Transportation Meteorology Key laboratory Nanjing Joint Institute for Atmospheric SciencesNanjing 210041China Heavy Rain and Drought-Flood Disasters in Plateau and Basin Key laboratory of Sichuan Province Institute of Plateau MeteorologyCMAChengdu 610072China State Key laboratory of Disaster Weather Chinese Academy of Meteorological SciencesBeijing 100081China Collaborative Innovation Center for Western Ecological Safety Lanzhou UniversityLanzhou 730000China China Meteorological Administration aerosol-Cloud and Precipitation Key laboratory and Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters(CIC-FEMD) Nanjing University of Information Science and TechnologyNanjing 210044China

The Sichuan-Xizang Railway is an important part of the railway network in China, and geological disasters, such as mountain floods and landslides, frequently occur in this region. Precipitation is an important cause of these disasters;therefore,accurate simulation of the precipitation in this region is highly important. In this study, the descriptions for uncertain processes in the cloud microphysics scheme are improved;these processes include cloud droplet activation, cloud-rain autoconversion, rain accretion by cloud droplets, and the entrainment-mixing process. In the default scheme, the cloud water content of different sizes corresponds to the same cloud droplet concentration, which is inconsistent with the actual content;this results in excessive cloud droplet size, unreasonable related conversion rates of microphysical process(such as cloud-rain autoconversion), and an overestimation of precipitation. Our new scheme overcomes the problem of excessive cloud droplet size. The processes of cloudrain autoconversion and rain accretion by cloud droplets are similar to the stochastic collection equation, and the mixing mechanism of cloud droplets is more consistent with that occurred during the actual physical process in the cloud. Based on the new and old schemes, multiple precipitation processes in the flood season of 2021 along the Sichuan-Xizang Railway are simulated, and the results are evaluated using ground observations and satellite data. Compared to the default scheme, the new scheme is more suitable for the simulation of cloud physics, reducing the simulation deviation of the liquid water path and droplet radius from 2 times to less than 1 time and significantly alleviating the overestimation of precipitation intensity and range of precipitation center. The average root-mean-square error is reduced by 22%. Our results can provide a scientific reference for improving precipitation forecasting and disaster prevention in this region.

关键词： The Sichuan-Xizang Railway Cloud microphysics Precipitation Model improvement

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The new challenges for the development of NH_(3)-SCR catalysts under new situation of energy transition in power generation industry

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Chinese Chemical Letters 2024年第6期35卷 95-103页

作者： Feibin Wei Yongfang Rao Yu Huang Wei Wang Hui Mei Science and Technology on Thermostructural Composite Materials laboratory School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Key laboratory of aerosol Chemistry and Physics State Key Laboratory of Loess and Quaternary Geology(SKLLQG)Institute of Earth EnvironmentChinese Academy of SciencesXi’an 710061China Center of Excellence in Quaternary Science and Global Change Chinese Academy of SciencesXi’an 710061China University of Chinese Academy of Sciences Beijing 100049China Department of Environmental Science and Engineering Xi’an Jiaotong UniversityXi’an 710049China

NH_(3)-SCR was one of the most promising de NO_x technologies and it has been widely applied in industrial NO_x reduction.However,with the further development of energy transformation in power generation sector,the development of NH_(3)-SCR catalysts is facing some new challenges.It is becoming an urgent problem to solve low catalytic activity and stability of NH_(3)-SCR catalysts at the working condition of ultra-low temperature(≤200℃)and high concentrations of H_(2)O+SO_(2) due to the gradual deployment of new energy power plants.Furthermore,the traditional coal-fired power plants would need flexible operation with the increasing share of renewable energy generation.The NH_(3)-SCR catalysts which were applied in coal-fired power industry would be requested to work in a wide temperature window from 200℃ to 500℃ in the near future.Therefore,in this review,we summarized the progress of NH_(3)-SCR catalysts in solving these different industrial problems in recent years.And the research directions which were deserved to be focused on the development of NH_(3)-SCR catalysts for the energy transition of power generation sector are proposed.

关键词： NH_(3)-SCR NOx reduction Power generation Ultra-low temperature Wide temperature windows

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Promoted surface charge density from interlayer Zn–N_(4) configuration in carbon nitride for enhanced CO_(2) photoreduction

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Nano Research 2024年第4期17卷 2400-2409页

作者： Xianjin Shi Yu Huang Gangqiang Zhu Wei Peng Meijuan Chen State Key laboratory of Loess and Quaternary Geology(SKLLQG) Key Laboratory of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi’an 710061China Center of Excellence in Quaternary Science and Global Change Chinese Academy of SciencesXi’an 710061China University of Chinese Academy of Sciences Beijing 100049China School of Physics and Information Technology Shaanxi Normal UniversityXi’an 710062China School of Human Settlements and Civil Engineering Xi’an Jiaotong UniversityXi’an 710049China

The solar-driven reduction of CO_(2) into valuable products is a promising method to alleviate global environmental problems and energy crises.However,the low surface charge density limits the photocatalytic conversion performance of CO_(2).Herein,a polymeric carbon nitride(PCN)photocatalyst with Zn single atoms(Zn1/CN)was designed and synthesized for CO_(2) photoreduction.The results of the CO_(2) photoreduction studies show that the CO and CH_(4) yields of Zn1/CN increased fivefold,reaching 76.9 and 22.9μmol/(g·h),respectively,in contrast to the unmodified PCN.Ar+plasma-etched X-ray photoelectron spectroscopy and synchrotron radiation-based X-ray absorption fine structure results reveal that Zn single atom is mainly present in the interlayer space of PCN in the Zn–N_(4) configuration.Photoelectrochemical characterizations indicate that the interlayer Zn–N_(4) configuration can amplify light absorption and establish an interlayer charge transfer channel.Light-assisted Kelvin probe force microscopy confirms that more photogenerated electrons are delivered to the catalyst surface through interlayer Zn–N_(4) configuration,which increases its surface charge density.Further,in-situ infrared spectroscopy combined with density functional theory calculation reveals that promoted surface charge density accelerates key intermediates(*COOH)conversion,thus achieving efficient CO_(2) conversion.This work elucidates the role of internal single atoms in catalytic surface reactions,which provides important implications for the design of single-atom catalysts.

关键词： single-atom catalysts photocatalytic CO_(2)reduction interlayer modification charge transfer dynamics surface charge density

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