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Observational and modelled insights of volatile organic compounds into seasonal atmospheric oxidation capacity and radical chemistry over North China 认领 引用
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作者 Gen Zhang Jiyun Xian +6 位作者 Xue Yang Ouyang Li Guolan Fan Jinhe Wang Zhiyong Xia Luhong Gao Yanmei Jiang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第5期48-58,共11页
Volatile organic compounds(VOCs)regulate secondary pollutant formation by controlling both atmospheric oxidation capacity(AOC)intensity and ROx cycling efficiency.However,their dynamic mechanisms under varying seasona... Volatile organic compounds(VOCs)regulate secondary pollutant formation by controlling both atmospheric oxidation capacity(AOC)intensity and ROx cycling efficiency.However,their dynamic mechanisms under varying seasonal and pollution conditions remain poorly understood.In this study,the seasonal variations in AOC and radical chemistry under contrasting pollution scenarios were quantified based on the synchronized measurements of VOCs and other trace gases in Jinan,China.Severe ozone pollution was identified in summer with 8 h average ozone(O3)levels exceeding the Chinese national ambient air quality on 22 days(or 73.3%in frequency).Winter haze episodes(38.7%in frequency)exhibited significant PM2.5accumulation alongside pronounced VOCs enhancement.VOCs exhibited marked seasonal divergence:summer pollution depleted alkanes(-23%)but enriched oxygenated VOCs(OVOCs,+28%)through photochemical processing,whereas winter conditions amplified primary VOCs emissions.AOC confirmed summer dominance,with an average value of 1.6×107molecules/(cm3·s),exceeding winter AOC values by 7-8 folds.OH reactivity analysis further distinguished seasonal drivers,with OVOCs accounting for 34%of summer OH depletion versus NO2/CO-dominated consumption(61.2%)in winter.HCHO/OVOCs photolysis contributed 65%-89%to HO2/RO2production in summer(54%-56%in winter),whilst OH generation primarily originated from HONO photolysis(38%-44%in winter)and O3dissociation(59%-74%in summer).Summer pollution episodes intensified radical cycling,as evidenced via accelerated summer OH production rates during pollution days. 展开更多
关键词 Volatile organic compounds(VOCs) Atmospheric oxidation capacity(AOC) OH reactivity O3 ROx radicals
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Atmospheric oxidation capacity and its influence on secondary pollution during winter PM2.5haze episodes in Urumqi 认领 引用
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作者 Binqian Fan Yingying Liu +5 位作者 Gaofeng Yu Zhenze Song Yanhui Liu Xiaoli Wang Chunmei Geng Wen Yang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第2期468-480,共13页
Atmospheric oxidation capacity(AOC)refers to the oxidation capacity of atmospheric chemical processes for major pollutants.A comprehensive observation campaign was conducted on a typical PM2.5pollution event in Uru... Atmospheric oxidation capacity(AOC)refers to the oxidation capacity of atmospheric chemical processes for major pollutants.A comprehensive observation campaign was conducted on a typical PM2.5pollution event in Urumqi,Northwest China,from January 15 to February 15,2024.Four typical cases representing PM2.5levels from non-polluted to heavily polluted periods were selected to estimate AOC,OH reactivity,their relationship with secondary components,and the HOxbudget in PM2.5using the Framework for 0-D Atmospheric Modeling model.Aromatics and alkanes contributed 54%-79%and 18%-46%of secondary organic aerosols(SOA)formation,respectively.The sulfur oxidation ratio(SOR)and nitrogen oxidation ratio(NOR)increased with rising PM2.5levels.As AOC increased,SOR showed the same trend,while NOR and SOA decreased slightly,and ammonia oxidation ratio values remained almost unchanged.OH radicals were the primary oxidants during the daytime,whereas NO3played a dominant role at nighttime.CO(24%-51%),NO2(27%-34%),and alkenes(7%-12%)were the dominant contributors to OH reactivity.The HO2+NO reaction pathway contributes 67%-84%to the production of OH,while Others(including carbonyl compounds photolysis,the permutation reactions of RO2,etc.),RO2+NO and OH+CO reaction pathways were the main pathways for HO2 production.A comprehensive understanding of the interactions among AOC,SOA,and radical cycling is crucial for formulating effective air quality management strategies aimed at mitigating secondary pollution under diverse atmospheric conditions. 展开更多
关键词 Secondary organic aerosols Atmospheric oxidation capacity Photochemical consumed VOCs OH reactivity HOx budget
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Atmospheric oxidation capacity and O3 formation in a coastal city of southeast China:Results from simulation based on four-season observation 认领 引用 被引量：3
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作者 Gaojie Chen Taotao Liu +9 位作者 Jinsheng Chen Lingling Xu Baoye Hu Chen Yang Xiaolong Fan Mengren Li Youwei Hong Xiaoting Ji Jinfang Chen Fuwang Zhang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2024年第2期68-80,共13页
The pollution of atmospheric ozone in China shows an obvious upward trend in the past decade.However,the studies on the atmospheric oxidation capacity and O3formation in four seasons in the southeastern coastal reg... The pollution of atmospheric ozone in China shows an obvious upward trend in the past decade.However,the studies on the atmospheric oxidation capacity and O3formation in four seasons in the southeastern coastal region of China with the rapid urbanization remain limited.Here,a four-season field observation was carried out in a coastal city of southeast China,using an observation-based model combining with the Master Chemical Mechanism,to explore the atmospheric oxidation capacity(AOC),radical chemistry,O3formation pathways and sensitivity.The results showed that the average net O3production rate(14.55 ppbv/hr)in summer was the strongest,but the average O3concentrations in autumn was higher.The AOC and ROx levels presented an obvious seasonal pattern with the maximum value in summer,while the OH reactivity in winter was the highest with an average value of 22.75 sec-1.The OH reactivity was dominated by oxygenated VOCs(OVOCs)(30.6%-42.8%),CO(23.2%-26.8%),NO2(13.6%-22.0%),and alkenes(8.4%-12.5%)in different seasons.HONO photolysis dominated OH primary source on daytime in winter,while in other seasons,HONO photolysis in the morning and ozone photolysis in the afternoon contributed mostly.Sensitivity analysis indicated that O3production was controlled by VOCs in spring,autumn and winter,but a VOC-limited and NOx-limited regime in summer,and alkene and aromatic species were the major controlling factors to O3formation.Overall,the study characterized the atmospheric oxidation capacity and elucidated the controlling factors for O3production in the coastal area with the rapid urbanization in China. 展开更多
关键词 Atmospheric oxidation capacity Radical chemistry Ozone production Sensitivity analysis
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Significant contribution of carbonyls to atmospheric oxidation capacity(AOC)during the winter haze pollution over North China Plain 认领 引用 被引量：5
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作者 Xue Yang Gen Zhang +4 位作者 Guang Pan Guolan Fan Houyong Zhang Xuan Ge Mingyue Du 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2024年第5期377-388,共12页
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... 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 elucidated.Here we measured carbonyl compounds and other trace gasses together with PM2.5over urban Jinan in North China Plain during the winter.Markedly 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 days.Results from observational-based model(OBM)with atmospheric oxidation capacity(AOC)indicated that AOC significantly increased with the increasing carbonyls during the winter haze events.Carbonyl photolysis have supplied key oxidants such as RO2 and HO2,and thereby enhancing the formation of fine particles and secondary organic aerosols,elucidating the observed haze-carbonyls inter-correlation.Diurnal 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 HCHO.This 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. 展开更多
关键词 Carbonyls Haze Observation-based model Source apportionment Atmospheric oxidation capacity
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Implications of 1.5 K climate warming on warm-season ozone exposure and atmospheric oxidation capacity in China 认领 引用
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作者 Zhihao Shi Lin Huang +5 位作者 Xiaodong Xie Momei Qin Jingyi Li Bingye Xu Lingling Jin Jianlin Hu 《Atmospheric and Oceanic Science Letters》 CSCD 2024年第6期53-61,共9页
Surface ozone(O3)poses significant threats to public health,agricultural crops,and plants in natural ecosystems.Global warming is likely to increase future O3mainly by altering atmospheric photochemical reaction... Surface ozone(O3)poses significant threats to public health,agricultural crops,and plants in natural ecosystems.Global warming is likely to increase future O3mainly by altering atmospheric photochemical reactions and enhancing biogenic volatile organic compound(BVOC)emissions.To assess the impacts of the future 1.5 K climate target on O3concentrations and ecological O3exposure in China,numerical simulations were conducted using the CMAQ(Community Multiscale Air Quality)model during April-October 2018.Ecological O3exposure was estimated using six indices(i.e.,M7,M24,N100,SUM60,W126,and AOT40f).The results show that the temperature rise increases the MDA8 O3(maximum daily eight-hour average O3)concentrations by∼3 ppb and the number of O3exceedance days by 10-20 days in the North China Plain(NCP),Yangtze River Delta(YRD),and Sichuan Basin(SCB)regions.All O3exposure indices show substantial increases.M24 and M7 in eastern and southern China will rise by 1-3 ppb and 2-4 ppb,respectively.N100 increases by more than 120 h in the surrounding regions of Beijing.SUM60 increases by greater than 9 ppm h−1,W126 increases by greater than 15 ppm h−1in Shaanxi and SCB,and AOT40f increases by 6 ppm h−1in NCP and SCB.The temperature increase also promotes atmospheric oxidation capacity(AOC)levels,with the higher AOC contributed by OH radicals in southern China but by NO3radicals in northern China.The change in the reaction rate caused by the temperature increase has a greater influence on O3exposure and AOC than the change in BVOC emissions. 展开更多
关键词 Temperature increase Ozone exposure Biogenic emissions Atmospheric oxidation capacity
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Future changes in ozone and oxidation capacity in China under the carbon peaking policy:The role of emissions and meteorology 认领 引用
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作者 Ao Shen Yiming Liu +3 位作者 Yuqi Zhu Xiao Lu Qi Fan Lei Li 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第7期504-515,共12页
Future ozone(O₃)pollution in China is shaped by complex interactions between emission reductions and meteorological changes under China’s carbon peaking and neutrality targets.This study employs the WRF-CMAQ modeling... Future ozone(O₃)pollution in China is shaped by complex interactions between emission reductions and meteorological changes under China’s carbon peaking and neutrality targets.This study employs the WRF-CMAQ modeling system with process analysis to quantify the impacts of meteorology and emissions on O₃and atmospheric oxidation capacity(AOC)across major Chinese regions in 2030.Under the carbon peaking scenario,wintertime O₃concentration increases across most regions,while summertime daytime O₃decreases except in the Yangtze River Delta(YRD).Nighttime O₃generally increases across all regions,and overall AOC is enhanced,particularly in summer.Disentangling the roles of meteorology and emissions shows that,although meteorological changes alone would reduce O₃in winter through enhanced dilution and limited photochemical activity,the effect of emission reductions dominates by weakening the nitric oxide(NO)titration effect,resulting in a net O₃increase.In summer,daytime emission reductions weaken NO titration,while higher humidity suppresses O₃formation,except in the YRD,where reduced humidity promotes O₃production.At night,stronger winds enhance vertical mixing and promote the downward transport of O₃from the residual layer,and the reduced NO titration effect further increases O₃levels.These findings underscore the importance of targeted mitigation strategies that account for the distinct seasonal and regional responses of O₃and AOC to both emission and meteorological changes under future climate and policy scenarios. 展开更多
关键词 Ozone Atmospheric oxidation capacity Carbon peaking policy WRF-CMAQ Process analysis
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The primary sources of ROx radicals in atmosphere:Oxidative capacity and self-purifying effect 认领 引用
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作者 Gaojie Chen Ziyi Lin +5 位作者 Xiaoting Ji Lingling Xu Xiaolong Fan Mengren Li Youwei Hong Jinsheng Chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第2期490-496,共7页
Ambient ozone(O3)is generated through the reactions of nitrogen oxides and volatile organic compounds(VOCs)in sunlight,and the primary sources of ROxradicals play a very important role in O3photochemistry.How... Ambient ozone(O3)is generated through the reactions of nitrogen oxides and volatile organic compounds(VOCs)in sunlight,and the primary sources of ROxradicals play a very important role in O3photochemistry.However,as major precursors of ROxradicals,the systematical evaluation of ClNO2,HCHO,and HONO impacts on O3photochemistry remains limited.Here,we utilized the observations of ClNO2,HCHO,and HONO conducted in a coastal city of Southeast China during a photochemical O3pollution episode,combined with model simulations to elucidate their impacts on ROxradicals and atmospheric oxidation capacity(AOC),as well as O3formation.Decreased concentrations of ClNO2and HONO were observed after sunrise,while HCHO concentrations peaked in the daytime.HCHO photolysis contributed the largest(∼25%)to ROxradical production around noon,while HONO photolysis(∼47%)dominated ROxradical production in the morning and late afternoon,and VOCs consumed by Cl radical released via ClNO2photolysis was more important(∼10%)in the early morning,similar to their effects on the AOC levels.The results of model simulations indicated that HCHO photolysis greatly enhanced the photochemical formation of O3,followed by HONO and ClNO2photolysis.Except for reducing VOCs due to a VOC-limited regime,the impacts of HCHO photolysis as primary ROxsources should be valued to inhibit the intensification of O3pollution.Our study stressed the importance of primary ROxsources for O3photochemistry in coastal regions,provided new insights into elucidating the self-purifying effect of the atmospheric environment. 展开更多
关键词 ROxradical chemistry O3photochemistry Atmospheric oxidation capacity Self-purifying effect
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Inconsistent capacity of potential HONO sources to enhance secondary pollutants:Evidence from WRF-Chem modeling 认领 引用
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作者 Jingwei Zhang Haiyan Ran +13 位作者 Yu Qu Chaofan Lian Weigang Wang Yusheng Zhang Feixue Zheng Xiaolong Fan Dawei Lu Chao Yan Kaspar RDaellenbach Zhiqiang Ma Yongchun Liu Maofa Ge Markku Kulmala Junling An 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2025年第12期812-830,共19页
Nitrous acid(HONO)is a crucial source of OH radicals in the troposphere,significantly enhancing secondary pollutants like secondary organic aerosols(SOA)and peroxyacetyl nitrates(PAN).While prior research has examined... Nitrous acid(HONO)is a crucial source of OH radicals in the troposphere,significantly enhancing secondary pollutants like secondary organic aerosols(SOA)and peroxyacetyl nitrates(PAN).While prior research has examined HONO sources and their total impacts on secondary pollution,the specific enhancement capacity of each individual HONO source remains underexplored.This study uses observational data from 2015 to 2018 for HONO,SOA,and PAN across six sites in China,combined with WRF-Chem model adding six potential HONO sources to evaluate their capacity:traffic emissions(E_traffic),soil emissions(E_soil),indoor-outdoor exchange(E_indoor),nitrate photolysis(P_nit),and NO2 heterogeneous reactions on aerosol and ground surfaces(Het_a,Het_g).The simulated HONO contributions near the ground in urban Beijing were:12%from NO+OH(default source),10%-20%from E_traffic,1%-12%from P_nit,2%-10%from Het_a,and 50%-70% from Het_g.For SOA and PAN,we calculated incremental contributions enhanced by each HONO source and derived enhancement ratios(ERs)normalized against HONO’s contribution:~7 for P_nit,~2 for Het_a,~0.9 for Het_g,~0.8 for E_soil,~0.3 for E_traffic,and~0.1 for E_indoor.HONO sources’capacity to enhance secondary pollutants varies,being larger for aerosol-related sources.Vertical analysis on HONO concentration,spatial distribution,ROx radical cycling rates,and OH enhancements revealed that aerosol-related HONO sources,especially P_nit,contribute more to secondary pollution.Future research should focus more on assessing real-world impacts of HONO sources,besides identifying their budgets.Additionally,uptake coefficient(γ)and nitrate photolysis frequency(Jnitrate)critically affect HONO and secondary pollutant formation,necessitating further investigations. 展开更多
关键词 Nitrous acid WRF-Chem Secondary organic aerosols Peroxyacetyl nitrate Atmospheric oxidation capacity Vertical profiles
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Atmospheric oxidizing capacity in autumn Beijing:Analysis of the O3 and PM2.5 episodes based on observation-based model 认领 引用 被引量：8
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作者 Chenhui Jia Shengrui Tong +8 位作者 Xinran Zhang Fangjie Li Wenqian Zhang Weiran Li ZhenWang Gen Zhang Guiqian Tang Zirui Liu Maofa Ge 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2023年第2期557-569,共13页
Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O3)and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AO... Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O3)and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AOC still remains uncertainty.In this study,a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing,where O3 and PM2.5 episodes had been experienced successively.The observation-based model(OBM)is used to quantify the AOC at O3 and PM2.5 episodes.The strong intensity of AOC is found at O3 and PM2.5 episodes,and hydroxyl radical(OH)is the dominating daytime oxidant for both episodes.The photolysis of O3 is main source of OH at O3 episode;the photolysis of nitrous acid(HONO)and formaldehyde(HCHO)plays important role in OH formation at PM2.5 episode.The radicals loss routines vary according to precursor pollutants,resulting in different types of air pollution.O3 budgets and sensitivity analysis indicates that O3 production is transition regime(both VOC and NOx-limited)at O3 episode.The heterogeneous reaction of hydroperoxy radicals(HO2)on aerosol surfaces has significant influence on OH and O3 production rates.The HO2 uptake coefficient(γHO2)is the determining factor and required accurate measurement in real atmospheric environment.Our findings could provide the important bases for coordinated control of PM2.5 and O3 pollution. 展开更多
关键词 Pollution episode Observation-based model Atmospheric oxidizing capacity Heterogeneous reaction Hydroxyl radical Budgets
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Progress in quantitative research on the relationship between atmospheric oxidation and air quality 认领 引用 被引量：3
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作者 Yuesi Wang Xin Jin +12 位作者 Zirui Liu Gehui Wang Guiqian Tang Keding Lu Bo Hu Shanshan Wang Guohui Li Xinqin An Chao Wang Qihou Hu Lingyan He Fenfen Zhang Yuanhang Zhang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2023年第1期350-366,共17页
Atmospheric oxidizing capacity(AOC)is an essential driving force of troposphere chemistry and self-cleaning,but the definition of AOC and its quantitative representation remain uncertain.Driven by national demand for ... Atmospheric oxidizing capacity(AOC)is an essential driving force of troposphere chemistry and self-cleaning,but the definition of AOC and its quantitative representation remain uncertain.Driven by national demand for air pollution control in recent years,Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research.This paper will give a brief review of these developments.First,AOC indexes were established that represent apparent atmospheric oxidizing ability(AOIe)and potential atmospheric oxidizing ability(AOIp)based on aspects of macrothermodynamics and microdynamics,respectively.A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing,and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country.In addition,the detection of ground or vertical profiles for atmospheric OH·,HO2·,NO3·radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments.Moreover,laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O3and NO2,which are typical oxidants in the surface/interface atmosphere,and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies,multiphase and multi-interface conditions were obtained.Finally,based on the GRAPES-CUACE adjoint model improved by Chinese scholars,simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized.Normalized numerical simulations of AOIe and AOIp were performed,and regional coordination of AOC was adjusted.An optimized plan for controlling O3and PM2.5was analyzed by scenario simulation. 展开更多
关键词 Atmospheric oxidizing capacity(AOC) Quantitative index Free radicals Observation and modeling Air quality
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Enhanced nitrous acid(HONO)formation via NO2uptake and its potential contribution to heavy haze formation during wintertime 认领 引用 被引量：3
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作者 Zirui Liu Rong Yang +6 位作者 Jingyun Liu Keding Lu Guiqian Tang Yuepeng Pan Dongsheng Ji Yuesi Wang Bo Hu 《Atmospheric and Oceanic Science Letters》 CSCD 2024年第6期15-20,共6页
full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban si... full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH3),and aerosol surface area,and the promotional effect of NH3for nitrogen dioxide(NO2)uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO2on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO2on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere. 展开更多
关键词 Nitrous acid Budget analysis Heterogeneous reactions of NO2 Heavy pollution episodes Atmospheric oxidation capacity
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NO_x Release from Snow and Ice Covered Surface in Polar Regions and the Tibetan Plateau 认领 引用 被引量：1
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作者 Feng Wang Weili Lin +1 位作者 Junxia Wang Tong Zhu 《Advances in Climate Change Research》 2011年第3期141-148,共8页
The exchanges of NOx between snow and air have significant impact on the atmospheric components and photochemical processes in the overlying boundary layer. Such exchanges increase the oxidizing capacity of the atmosp... The exchanges of NOx between snow and air have significant impact on the atmospheric components and photochemical processes in the overlying boundary layer. Such exchanges increase the oxidizing capacity of the atmosphere and may have a crucial impact on the air signals that are retrieved from ice cores. In the recent years, sunlit snow and ice have been demonstrated to be important NOx sources in the polar atmospheric boundary layer. This paper makes a thorough review on the release of NOx from snow and ice, including field observations and experimental evidences, release mechanisms and influential parameters that affect such a release process, polar NOx concentrations and fluxes, and environmental impacts of the chemical processes of NOx in the polar atmospheric boundary layer. In the Tibetan Plateau, the released NOx observed recently in the sunlit snow/ice-cover is 1-order magnitude more than that in polar regions, but further scientific research is still needed to reveal its impact on the atmospheric oxidizing capacity. 展开更多
关键词 NOx exchange between snow and air polar area atmospheric oxidizing capacity Tibetan Plateau
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Reactions with Criegee intermediates are the dominant gas-phase sink for formyl fluoride in the atmosphere 认领 引用 被引量：2
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作者 Yu Xia Bo Long +1 位作者 Ai Liu Donald G.Truhlar 《Fundamental Research》 CAS CSCD 2024年第5期1216-1224,共9页
Atmospheric oxidation processes are of central importance in atmospheric climate models.It is often considered that volatile organic molecules are mainly removed by hydroxyl radical;however,the kinetics of some reacti... Atmospheric oxidation processes are of central importance in atmospheric climate models.It is often considered that volatile organic molecules are mainly removed by hydroxyl radical;however,the kinetics of some reactions of hydroxyl radical with volatile organic molecules are slow.Here we report rate constants for rapid reactions of formyl fluoride with Criegee intermediates.These rate constants are calculated by dual-level multistructural canonical variational transition state theory with small-curvature tunneling(DL-MS-CVT/SCT).The treatment contains beyond-CCSD(T)electronic structure calculations for transition state theory,and it employs validated density functional input for multistructural canonical variational transition state theory with small-curvature tunneling and for variable-reaction-coordinate variational transition state theory.We find that the M11-L density functional has higher accuracy than CCSD(T)/CBS for the HC(O)F+CH2OO and HC(O)F+anti-CH3CHOO reactions.We find significant negative temperature dependence in the ratios of the rate constants for HC(O)F+CH2OO/anti-CH3CHOO to the rate constant for HC(O)F+OH.We also find that different Criegee intermediates have different rate-determining-steps in their reactions with formyl fluoride,and we find that the dominant gas-phase removal mechanism for HC(O)F in the atmosphere is the reaction with CH2OO and/or anti-CH3CHOO Criegee intermediates. 展开更多
关键词 Atmospheric oxidation capacity Criegee intermediates Formyl fluoride Reaction kinetics CCSDT(Q)/CBS calculations
Response of organic aerosol characteristics to emission reduction in Yangtze River Delta region 认领 引用 被引量：5
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作者 Jinbo Wang Jiaping Wang +10 位作者 Wei Nie Xuguang Chi Dafeng Ge Caijun Zhu Lei Wang Yuanyuan Li Xin Huang Ximeng Qi Yuxuan Zhang Tengyu Liu Aijun Ding 《Frontiers of Environmental Science & Engineering》 SCIE EI CSCD 2023年第9期221-232,共12页
Organic aerosol(OA)is a major component of atmospheric particulate matter(PM)with complex composition and formation processes influenced by various factors.Emission reduction can alter both precursors and oxidants whi... Organic aerosol(OA)is a major component of atmospheric particulate matter(PM)with complex composition and formation processes influenced by various factors.Emission reduction can alter both precursors and oxidants which further affects secondary OA formation.Here we provide an observational analysis of secondary OA(SOA)variation properties in Yangtze River Delta(YRD)of eastern China in response to large scale of emission reduction during Chinese New Year(CNY)holidays from 2015 to 2020,and the COVID-19 pandemic period from January to March,2020.We found a 17%increase of SOA proportion during the COVID lockdown.The relative enrichment of SOA is also found during multi-year CNY holidays with dramatic reduction of anthropogenic emissions.Two types of oxygenated OA(OOA)influenced by mixed emissions and SOA formation were found to be the dominant components during the lockdown in YRD region.Our results highlight that these emission-reduction-induced changes in organic aerosol need to be considered in the future to optimize air pollution control measures. 展开更多
关键词 Emission control Secondary organic aerosol Atmospheric oxidizing capacity Holiday effects COVID-19 lockdown
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