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Growth of nitrate contribution to aerosol pollution during wintertime in Xi'an,northwest China:Formation mechanism and effects of NH_(3)

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Particuology 2024年第4期87卷 303-315页

作者： Hui Su Ting Zhang Suixin Liu Yao Qu Huan Li Jiamao Zhou Zhuzi Zhao Qiyuan Wang Lu Li Minxia Shen Shuoyuan Chen Steven Sai Hang Ho Junji Cao State key laboratory of Loess and Quaternary Geology.key laboratory ofAerosol Chemistry and Plhysics Institute of Earth EnvironmentChinese Acadery of SciencesXi'an 710061China Xi'an Institute for Innovative Earth Environment Research Xi'an 710061China National pbservation and Research Station of Regional Ecological Environment Change and Cornprehensive Management in the Guanzhong Plain Xi'an 710061China shaanxi key laboratory of atmospheric and haze fog pollution prevention Institute of Earth EnvironmentChinese Academy of SciencesXi'an 710061China University of Chinese Academy of Sciences Beijing 100049China School of Chemical and Environmental Engineering Jiangsu University of TechnologyChangzhou 213001China Division of atmospheric Sciences Desert Research InstituteReno NV89512United States Institute of atmospheric Physics Chinese Academy of SciencesBeijing 100029China

With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,*** further gain insights into the factors on nitrate formation and efficiently mitigate air pollution,highly time-resolved observations of water-soluble inorganic ions(WSIIs)in PM_(2.5) were measured in a suburban area of Xi'an,China during *** concentration of total WSIIs is 39.8μg m-3 on average,accounting for 50.3%of PM_(2.5) *** contrast to a slight decrease in the mass fraction of SO_(4)^(2-),NO_(3)-shows a sig-nificant increase of the PM_(2.5) contribution with the aggravation of aerosol *** suggests the importance of NO_(3)-formation to haze ***,homogeneous reactions govern the formation of NO_(3)-,while alkali metals such as calcium and sodium play an additional role in retaining NO_(3)-in PM_(2.5) during clean ***,the heterogeneous hydrolysis reaction contributed more to NO_(3)-formation during the pollution periods under high relative *** investigation reveals that temperature,relative humidity,oxidant,and ammonia emissions facilitate rapid NO_(3)-*** the random forest(RF)model,NO_(3)-concentrations were successfully simulated with measured variables for the training and testing datasets(R2>0.95).Among these variables,CO,NH_(3),and NO_(2) were found to be the main factors affecting the NO_(3)-*** with the period without vehicle re-striction,the contributions of NO_(3)-and NH4+to PM_(2.5) mass decreased by 5.3%and 3.4%in traffic re-striction periods,*** vehicle restriction leads to the decreases of precursor gases of NO_(2),SO_(2),and NH_(3) by 12.8%,5.9%,and 27.6%,*** results demonstrate collaborative emission reduction of NO_(x) and NH_(3) by vehicle restrictions,and using new energy vehicles(or electric vehicles)can effectively alleviate particul

关键词： PM_(2.5) Water-soluble inorganic ions Nitrate formation Excess ammonium Vehicle restrictions

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Significant contribution of carbonyls to atmospheric oxidation capacity(AOC)during the winter haze pollution over North China Plain

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Journal of Environmental Sciences 2024年第5期139卷 377-388页

作者： Xue Yang Gen Zhang Guang Pan Guolan Fan Houyong Zhang Xuan Ge Mingyue Du School of Municipal and Environmental Engineering Shandong Jianzhu UniversityJi’nan 250101China State key laboratory of Severe Weather&key laboratory of atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological SciencesBeijing 100081China Shandong Jinan Ecological Environment Monitoring Center Ji’nan 250101China

atmospheric carbonyl compounds play significant roles in the cycling of radicals and have exhibited surprisingly high levels in winter that were well correlated to particulate matter,for which the reason have not been clearly *** we measured carbonyl compounds and other trace gasses together with PM_(2.5)over urban Jinan in North China Plain during the *** higher carbonyl concentrations(average:14.63±4.21 ppbv)were found during wintertime haze pollution,about one to three-times relative to those on nonhaze days,with slight difference in chemical composition except formaldehyde(HCHO).HCHO(3.68 ppbv),acetone(3.17 ppbv),and acetaldehyde(CH_3CHO)(2.83 ppbv)were the three most abundant species,accounting for~75% of the total carbonylson both haze and non-haze *** from observational-based model(OBM)with atmospheric oxidation capacity(AOC)indicated that AOC significantly increased with the increasing carbonyls during the winter haze *** photolysis have supplied key oxidants such as RO_(2) and HO_(2),and thereby enhancing the formation of fine particles and secondary organic aerosols,elucidating the observed haze-carbonyls *** variation with carbonyls exhibiting peak values at early-noon and night highlighted the combined contribution of both secondary formation and primary diesel-fuel sources.1-butene was further confirmed to be the major precursor for *** study confirms the great contribution of carbonyls to AOC,and also suggests that reducing the emissions of carbonyls would be an effective way to mitigate haze pollution in urban area of the NCP region.

关键词： Carbonyls haze Observation-based model Source apportionment atmospheric oxidation capacity

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燃烧源氨排放对灰霾期间北京大气铵的重要贡献

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Science Bulletin 2024年第7期69卷 978-987页

作者：吴礼彬王芃张强任红 Zongbo Shi 胡伟陈静谢巧蓉李林杰越思瑶韦莲芳宋琳琳张永根王子涵陈爽韦琬王小曼章炎麟孔少飞葛宝珠杨婷方运霆任露洁邓君俊孙业乐王自发张宏亮胡建林刘丛强 Roy M.Harrison Qi Ying 傅平青 Institute of Surface-Earth System Science School of Earth System ScienceTianjin UniversityTianjin 300072China Department of atmospheric and Oceanic Sciences Fudan UniversityShanghai 200438China IRDR ICoE on Risk Interconnectivity and Governance on Weather/Climate Extremes Impact and Public Health Fudan UniversityShanghai 200438China Ministry of Education key laboratory for Earth System Modeling Department of Earth System ScienceTsinghua UniversityBeijing 100084China Air Environmental Modeling and pollution Controlling key laboratory of Sichuan Higher Education Institute Chengdu University of Information TechnologyChengdu 610225China Division of Environmental Health&Risk Management School of GeographyEarth&Environmental SciencesUniversity of BirminghamBirmingham B152TTUK School of Environmental Science and Engineering Tianjin UniversityTianjin 300072China State key laboratory of atmospheric Boundary Layer Physics and atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China key laboratory of Forest Ecology and Management Institute of Applied EcologyChinese Academy of SciencesShenyang 110164China Yale-NUIST Center on atmospheric Environment International Joint Laboratory on Climate and Environment ChangeNanjing University of Information Science and TechnologyNanjing 210044China Department of atmospheric Sciences School of Environmental Studies and Department of Environmental Science and TechnologySchool of Environmental StudiesChina University of GeosciencesWuhan 430074China Department of Environmental Science and Engineering Fudan UniversityShanghai 200438China Collaborative Innovation Center of atmospheric Environment and Equipment Technology Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution ControlNanjing University of Information Science and TechnologyNanjing 210044China Department of Environmental Sciences/Center of Excellence in Environmental Studies King Abdulaziz UniversityJeddah 21589Saudi Arabia Zachr

Aerosol ammonium(NH_(4)^(+)),mainly produced from the reactions of ammonia(NH_(3))with acids in the atmosphere,has significant impacts on air pollution,radiative forcing,and human *** the source and formation mechanism of NH_(4)^(+)can provide scientific insights into air quality ***,the sources of NH_(3)in urban areas are not well understood,and few studies focus on NH_(3)/NH_(4)^(+)at different heights within the atmospheric boundary layer,which hinders a comprehensive understanding of aerosol NH_(4)^(+).In this study,we perform both field observation and modeling studies(the Community Multiscale Air Quality,CMAQ)to investigate regional NH_(3)emission sources and vertically resolved NH_(4)^(+)formation mechanisms during the winter in *** stable nitrogen isotope analyses and CMAQ model suggest that combustion-related NH_(3)emissions,including fossil fuel sources,NH_(3)slip,and biomass burning,are important sources of aerosol NH_(4)^(+)with more than 60%contribution occurring on heavily polluted *** contrast,volatilization-related NH_(3)sources(livestock breeding,N-fertilizer application,and human waste)are dominant on clean ***-related NH_(3)is mostly local from Beijing,and biomass burning is likely an important NH_(3)source(~15%–20%)that was previously *** effective control strategies such as the two-product(e.g.,reducing both SO_(2)and NH_(3))control policy should be considered to improve air quality.

关键词： Particulate ammonium Nitrogen isotope PM2.5 The Community Multiscale Air Quality(CMAQ) Control policy

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Quantum key distribution over a mimicked dynamic-scattering channel

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Science China(Information Sciences) 2024年第4期67卷 323-330页

作者： Qi-Hang LU Fang-Xiang WANG Wei CHEN Hai-Yang FU Yin-Jie LU Shuang WANG De-Yong HE Zhen-Qiang YIN Guang-Can GUO Zheng-Fu HAN CAS key laboratory of Quantum Information University of Science and Technology of China CAS Center for Excellence in Quantum Information and Quantum Physics University of Science and Technology of China Hefei National laboratory University of Science and Technology of China

Free-space quantum key distribution(QKD) plays an important role in the global quantum network. However, free space channels suffer from the atmospheric turbulence and scattering effects of haze,fog, and dust, which significantly weaken the performance of QKD or even block the secure quantum ***, we prove the performance of QKD over a dynamic scattering channel can be enhanced significantly using a fast wavefront shaping technique. The system achieves on average 10-dB enhancement of quantum transmission efficiency and establishes a secure quantum link for QKD. Our work demonstrates the feasibility of QKD through free-space dynamic scattering channels and enhances the deployment capability of complex-channel QKD system.

关键词： quantum key distribution free space channel channel turbulence channel scattering wavefront shaping

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A critical review of sulfate aerosol formation mechanisms during winter polluted periods

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Journal of Environmental Sciences 2023年第1期123卷 387-399页

作者： Can Ye Keding Lu Huan Song Yujing Mu Jianmin Chen Yuanhang Zhang State key Joint laboratory of Environmental Simulation and pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China Shanghai key laboratory of atmospheric Particle pollution and prevention Department of Environmental Science and EngineeringInstitute of Atmospheric SciencesFudan UniversityShanghai 200438China

Sulfate aerosol contributes to particulate matter pollution and plays a key role in aerosol radiative forcing,impacting human health and climate *** models tend to substantially underestimate sulfate concentrations during haze episodes,indicating that there are still missing mechanisms not considered by the *** recent good progress in understanding the missing sulfate sources,knowledge on different sulfate formation pathways during polluted periods still involves large uncertainties and the dominant mechanism is under heated debate,calling for more field,laboratory,and modeling ***,we review the traditional sulfate formation mechanisms in cloud water and also discuss the potential factors affecting multiphase S(Ⅳ)*** recent progress in multiphase S(Ⅳ)oxidation mechanisms is *** formation rates by different prevailing oxidation pathways under typical winter-haze conditions are also calculated and *** on the literature reviewed,we put forward control of the atmospheric oxidation capacity as a means to abate sulfate aerosol ***,we conclude with a concise set of research priorities for improving our understanding of sulfate formation mechanisms during polluted periods.

关键词： Sulfate aerosol Formation mechanisms Multiphase oxidation Transition metal ions Reactive oxygen species

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Application of smog chambers in atmospheric process studies

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National Science Review 2022年第2期9卷 126-141页

作者： Biwu Chu Tianzeng Chen Yongchun Liu Qingxin Ma Yujing Mu Yonghong Wang Jinzhu Ma Peng Zhang Jun Liu Chunshan Liu Huaqiao Gui Renzhi Hu Bo Hu Xinming Wang Yuesi Wang Jianguo Liu Pinhua Xie Jianmin Chen Qian Liu Jingkun Jiang Junhua Li Kebin He Wenqing Liu Guibin Jiang Jiming Hao Hong He State key laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental Sciences Chinese Academy of Sciences State key Joint laboratory of Environment Simulation and pollution Control School of Environment Tsinghua University State key Joint laboratory of Environment Simulation and pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Center for Excellence in Regional atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences College of Resources and Environment University of Chinese Academy of Sciences Aerosol and haze laboratory Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing Convenient Environmental Tech Co.Ltd key laboratory of Environmental Optics and Technology Anhui Institutes of Optics and Fine Mechanics Chinese Academy of Sciences State key laboratory of atmospheric Boundary Layer Physics and atmospheric Chemistry Institute of Atmospheric Physics Chinese Academy of Sciences State key laboratory of Organic Geochemistry and Guangdong Provincial key laboratory of Environmental Protection and Resources Utilization Guangzhou Institute of Geochemistry Chinese Academy of Sciences Shanghai key laboratory of atmospheric Particle pollution and prevention Department of Environmental Science and Engineering Fudan University

Smog chamber experimental systems,which have been widely used in laboratory simulation for studying atmospheric processes,are comprehensively reviewed in this *** components,development history,main research topics and main achievements of smog chambers are *** smog chambers in the world,including their volumes,wall materials,light sources and features,are summarized and *** factors of smog chambers and their influences on the simulation of the atmospheric environment are discussed,including wall loss,wall emission and background *** features of next-generation smog chambers and their application prospect in future studies of the atmospheric environment are also outlined in this paper.

关键词： smog chamber simulation wall effect secondary aerosol ozone

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The missing base molecules in atmospheric acid-base nucleation

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National Science Review 2022年第10期9卷 196-208页

作者： Runlong Cai Rujing Yin Chao Yan Dongsen Yang Chenjuan Deng Lubna Dada Juha Kangasluoma Jenni Kontkanen Roope Halonen Yan Ma Xiuhui Zhang Pauli Paasonen Tuukka Pet?j? Veli-Matti Kerminen Yongchun Liu Federico Bianchi Jun Zheng Lin Wang Jiming Hao James N.Smith Neil M. Donahue Markku Kulmala Douglas R.Worsnop Jingkun Jiang Center for atmospheric Particle Studies Carnegie Mellon University Department of Chemistry Carnegie Mellon University Aerodyne Research Inc. State key Joint laboratory of Environment Simulation and pollution Control School of Environment Tsinghua University Institute for atmospheric and Earth System Research/Physics Faculty of Science University of Helsinki Aerosol and haze laboratory Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Collaborative Innovation Center of atmospheric Environment and Equipment Technology Nanjing University of Information Science and Technology laboratory of atmospheric Chemistry Paul Scherrer Institute Center for Joint Quantum Studies and Department of Physics School of Science Tianjin University key laboratory of Cluster Science Ministry of Education of China School of Chemistry and Chemical Engineering Beijing Institute of Technology Shanghai key laboratory of atmospheric Particle pollution and prevention (LAP3) Department of Environmental Science and Engineering Fudan University Chemistry Department University of California

Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration,cloud formation and hence the *** clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the ***,the acid-base cluster composition,measured using state-of-the-art mass spectrometers,cannot explain the measured high formation rate of new *** we present strong evidence for the existence of base molecules such as amines in the smallest atmospheric sulfuric acid clusters prior to their detection by mass *** demonstrate that forming(H2SO4)1(amine)1is the rate-limiting step in atmospheric H2SO4-amine nucleation and the uptake of(H2SO4)1(amine)1is a major pathway for the initial growth of *** proposed mechanism is very consistent with measured new particle formation in urban Beijing,in which dimethylamine is the key base for H2SO4nucleation while other bases such as ammonia may contribute to the growth of larger *** findings further underline the fact that strong amines,even at low concentrations and when undetected in the smallest clusters,can be crucial to particle formation in the planetary boundary layer.

关键词： acid-base nucleation aerosol new particle formation polluted urban environment

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COATS:Comprehensive observation on the atmospheric boundary layer three-dimensional structure during haze pollution in the North China Plain

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Science China Earth Sciences 2023年第5期66卷 939-958页

作者： Qianhui LI Hongsheng ZHANG Xiaoye ZHANG Xuhui CAI Xipeng JIN Lu ZHANG Yu SONG Ling KANG Fei HU Tong ZHU Tianjin key laboratory for Oceanic Meteorology Tianjin Meteorological Service CenterTianjin Meteorological BureauTianjin 300074China laboratory for Climate and Ocean-Atmosphere Studies Department of Atmospheric and Oceanic SciencesSchool of PhysicsPeking UniversityBeijing 100871China State key laboratory of Severe Weather and key laboratory of atmospheric Chemistry of CMA Chinese Academy of Meteorological SciencesChina Meteorological Administration(CMA)Beijing 100081China State key Joint laboratory of Environmental Simulation and pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China State key laboratory of atmospheric Boundary Layer Physics and atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China

The North China Plain(NCP)is troubled by severe haze pollution and the evolution of haze pollution is closely related to the atmospheric boundary layer(ABL).However,experimental and theoretical studies on the physical-chemical processes of the ABL in the NCP are lacking,with many scientific problems to be *** solve these problems,the Comprehensive Observation on the atmospheric boundary layer Three-dimensional Structure(COATS)during haze pollution was carried out in the NCP from 2016 to *** COATS experiment adopted a"point-line-surface"spatial layout,obtaining both spatial-temporal profiles of the meteorological and environmental elements in the ABL and the turbulent transport data of fine particulate matter(PM_(2.5))in winter and *** research achievements are as *** spatial-temporal distribution characteristics of the ABL structure and PM_(2.5)concentrations in NCP were *** typical thermal structure of persistent heavy haze events and the pollutant removal mechanism by low-level jets were *** was determined that the spatial structure of the ABL adjusted by the Taihang Mountains is responsible for the heterogeneous distribution of haze pollution in the NCP,and that mountain-induced vertical circulations can promote the formation of elevated pollution *** restraints of the atmospheric internal boundaries on horizontal diffusion of pollutants were *** contribution of the ABL to haze pollution in winter and summer was qualitatively compared and quantitatively *** turbulent transport nature behind the relationship between the atmospheric boundary layer height(ABLH)and surface PM_(2.5)concentrations was *** concept of"aerosol accumulation layer"was defined,and the applicability of the material method in determining ABLH was clarified.A measurement system for obtaining the turbulent flux of PM_(2.5)concentrations was developed,and the turbulence characteristics of PM_(2.5)concentrations w

关键词： COATS experiment haze pollution ABL three-dimensional structure Aerosol accumulation layer Turbulent flux of PM_(2.5)concentrations North China Plain

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Control of fine particulate nitrate during severe winter haze in“2+26”cities

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Journal of Environmental Sciences 2024年第2期136卷 261-269页

作者： Chuang Qin Xiao Fu Tao Wang Jian Gao Jiaqi Wang Institute of Environment and Ecology Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China Department of Civil and Environmental Engineering Hong Kong Polytechnic UniversityHong Kong 99907China State key laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 10084China

The“2+26”cities,suffering the most severe winter haze pollution,have been the key region for air quality improvement in *** prominent nitrate pollution is one of the most challenging environmental issues in this region,necessitating development of an effective control ***,we use observations,and state-of-the-art model simulations with scenario analysis and process analysis to quantify the effectiveness of the future SO_(2)-NO_(X)-VOC-NH_(3) emission control on nitrate pollution mitigation in“2+26”*** on a serious winter haze episode,we find that limited NO_(X)emission reduction alone in the short-term period is a less effective choice than VOC or NH_3emission reduction alone to decrease nitrate concentrations,due to the accelerated NO_(X)-HNO_(3)conversion by atmospheric oxidants and the enhanced HNO_(3)to NO_(3)^(-)partition by ammonia,although deep NO_(X)emission reduction is essential in the long-term *** synergistic NH_(3) and VOC emission control is strongly recommended,which can counteract the adverse effects of nonlinear photochemistry and aerosol chemical feedback to decrease nitrate *** extra benefits will be reduced if the synergistic NH_(3) and VOC reduction is delayed,and thus reducing emission of multiple precursors is urgently required for the effective control of increasingly severe winter nitrate pollution in“2+26”cities.

关键词： Nitrate Winter haze pollution Emission reduction “2+26”cities

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Chemical characterization and source identification of PM_(2.5) in Luoyang after the clean air actions

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Journal of Environmental Sciences 2022年第5期34卷 265-276页

作者： Min Xu Zirui Liu Bo Hu Guangxuan Yan Jianan Zou Shuman Zhao Jingxiang Zhou Xianhui Liu Xueping Zheng Xiaoyan Zhang Jing Cao Mengshuang Guan Yirong Lv Yanyun Zhang State key laboratory of atmospheric Boundary Layer Physics and atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China University of the Chinese Academy of Sciences Beijing 100049China key laboratory for Yellow River and Huai River Water Environment and pollution Control Henan Key Laboratory for Environmental Pollution ControlSchool of EnvironmentHenan Normal UniversityXinxiang 453007China Luoyang Eco-Environmental Monitoring Center of Henan Province Luoyang 471002China Luoyang Radiation Environment Service Office Luoyang 471002China 3 Clear Science&Technology Co. LtdBeijing 100029China

Luoyang is a typical heavy industrial city in China,with a coal-dominated energy structure and serious air *** the implementation of the clean air actions,the physic-ochemical characteristics and sources of PM_(2.5) have changed.A comprehensive study of PM_(2.5) was conducted from October 16,2019 to January 23,2020 to evaluate the effectiveness of previous control measures and further to provide theory basis for more effective policies in the *** showed that the aerosol pollution in Luoyang in autumn and win-ter is still serious with the average concentration of 91.1 μg/m^(3),although a large reduction(46.9%)since *** the contribution of nitrate increased from 12.5%to 25.1%and sul-fate decreased from 16.7%to 11.2%,aerosol pollution has changed from sulfate-dominate to *** NO_(3)^(-)/SO_(4)^(2-)ratio and the increasing of NO_(3)^(-)/SO_(4)^(2-)ratio with the aggravation of pollution indicating vehicle exhaust playing an increasingly important role in PM_(2.5) pollution in Luoyang,especially in the haze *** inorganic ions contributed significantly to the enhancement of PM_(2.5) during the pollution *** high value of Cl^(-)/Na^(+)and EC concentration indicate coal combustion in Luoyang is still *** top three contributor sources were secondary inorganic aerosols(33.3%),coal combus-tion(13.6%),and industrial emissions(13.4%).Close-range transport from the western and northeastern directions were more important factors in air pollution in Luoyang during the sampling *** is necessary to strengthen the control of coal combustion and reduce vehicle emissions in future policies.

关键词： Luoyang PM_(2.5) Chemical composition Source apportionment

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