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A review of gas-phase chemical mechanisms commonly used in atmospheric chemistry modelling

Journal of Environmental Sciences 2023年第1期123卷 522-534页

作者： Yanhui Liu Jiayin Li Yufang Ma Ming Zhou Zhaofeng Tan Limin Zeng Keding Lu Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Science and EngineeringPeking UniversityBeijing 100871China Institute of Energy and Climate Research IEK-8:TroposphereForschungszentrum Jülich GmbHJülich 52428Germany

The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of *** the first tropospheric chemical mechanism was proposed in the 1960s,various mechanisms including Master Chemical Mechanism(MCM),Carbon Bond Mechanism(CBM),Statewide Air Pollution Research Center(SAPRC)and Regional atmospheric chemistry Mechanism(RACM)have been developed for different research *** work summarizes the development and applications of these mechanisms,introduces their compositions and lumping methods,and compares the ways the mechanisms treat radicals with box model *** can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM,whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in *** photolysis rates of some oxygenated compounds are low in SAPRC07,which may result in underestimation of radical *** an explicit chemical mechanism,MCM describes the chemical processes of primary pollutants and their oxidation products in *** can be used to investigate certain chemical processes;however,due to its large size,it is rarely used in regional model simulations.A box model case study showed that the chemical behavior of OH and HO_(2)radicals and the production of ozone were well described by all *** and SAPRC underestimated the radical levels for different chemical treatments,leading to low ozone production values in both *** and RACM are widely used in box model studies,while CBM and SAPRC are often selected in regional simulations.

关键词： atmospheric chemistry Gas-phase chemical mechanism Ozone Box model

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Recent Progress in atmospheric chemistry Research in China: Establishing a Theoretical Framework for the “Air Pollution Complex”

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Advances in atmospheric Sciences 2023年第8期40卷 1339-1361页

作者： Tong ZHU Mingjin TANG Meng GAO Xinhui BI Junji CAO Huizheng CHE Jianmin CHEN Aijun DING Pingqing FU Jian GAO Yang GAO Maofa GE Xinlei GE Zhiwei HAN Hong HE Ru-Jin HUANG Xin HUANG Hong LIAO Cheng LIU Huan LIU Jianguo LIU Shaw Chen LIU Keding LU Qingxin MA Wei NIE Min SHAO Yu SONG Yele SUN Xiao TANG Tao WANG Tijian WANG Weigang WANG Xuemei WANG Zifa WANG Yan YIN Qiang ZHANG Weijun ZHANG Yanlin ZHANG Yunhong ZHANG Yu ZHAO Mei ZHENG Bin ZHU Jiang ZHU Peking University Beijing 100871China Guangzhou Institute of Geochemistry Chinese Academy of SciencesGuangzhou 510640China Hong Kong Baptist University Hong Kong SARChina Institute of atmospheric Physics Chinese Academy of SciencesBeijing 100029China Chinese Academy of Meteorological Sciences Beijing 100081China Fudan University Shanghai 200438China Nanjing University Nanjing 210023China Tianjin University Tianjin 300072China Chinese Research Academy of Environmental Sciences Beijing 100012China Ocean University of China Qingdao 266100China Institute of chemistry Chinese Academy of SciencesBeijing 100190China Nanjing University of Information Science and Technology Nanjing 210044China Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China Institute of Earth Environment Chinese Academy of SciencesXi’an 710061China University of Science and Technology of China Hefei 230026China Tsinghua University Beijing 100084China Anhui Institute of Optics and Fine Mechanics Hefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China Jinan University Guangzhou 510632China Hong Kong Polytechnic University Hong Kong SARChina Beijing Institute of Technology Beijing 100081China

atmospheric chemistry research has been growing rapidly in China in the last 25 years since the concept of the“air pollution complex”was first proposed by Professor Xiaoyan TANG in *** papers published in 2021 on air pollution(only papers included in the Web of Science Core Collection database were considered),more than 24000 papers were authored or co-authored by scientists working in *** this paper,we review a limited number of representative and significant studies on atmospheric chemistry in China in the last few years,including studies on(1)sources and emission inventories,(2)atmospheric chemical processes,(3)interactions of air pollution with meteorology,weather and climate,(4)interactions between the biosphere and atmosphere,and(5)data *** intention was not to provide a complete review of all progress made in the last few years,but rather to serve as a starting point for learning more about atmospheric chemistry research in *** advances reviewed in this paper have enabled a theoretical framework for the air pollution complex to be established,provided robust scientific support to highly successful air pollution control policies in China,and created great opportunities in education,training,and career development for many graduate students and young *** paper further highlights that developing and low-income countries that are heavily affected by air pollution can benefit from these research advances,whilst at the same time acknowledging that many challenges and opportunities still remain in atmospheric chemistry research in China,to hopefully be addressed over the next few decades.

关键词： atmospheric chemistry air pollution complex theoretical framework recent progress

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Some advances in atmospheric chemistry

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Progress in Natural Science:Materials International 2001年第9期 3-11页

作者：王明星杨昕 Beijing 100029 China Chinese Academy of Sciences Institute of atmospheric Physics State Key Laboratory of atmospheric Boundary Layer Physics and atmospheric chemistry

In the recent decade, researches have been carried out by our group on some aspects of atmospheric chemistry through field observation, mechanism analysis and model simulation. Here some main results on greenhouse gas (CH,, N20) emission from Chinese agricultural fields, aerosol, global carbon cycle and ozone variation in surface layer over China are briefly reported.

关键词： atmospheric chemistry methane aerosol carbon cycle surface ozone.

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Uncovering the dominant contribution of intermediate volatility compounds in secondary organic aerosol formation from biomass-burning emissions

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National Science Review 2024年第3期11卷 150-158页

作者： Kun Li Jun Zhang David M.Bell Tiantian Wang Houssni Lamkaddam Tianqu Cui Lu Qi Mihnea Surdu Dongyu Wang Lin Du Imad El Haddad Jay G.Slowik Andre S.H.Prevot Environment Research Institute Shandong University Laboratory of atmospheric chemistry Paul Scherrer Institute

Organic vapors from biomass burning are a major source of secondary organic aerosols(SOAs). Previous smog chamber studies found that the SOA contributors in biomass-burning emissions are mainly volatile organic compounds(VOCs). While intermediate volatility organic compounds(IVOCs) are efficient SOA precursors and contribute a considerable fraction of biomass-burning emissions, their contribution to SOA formation has not been directly observed. Here, by deploying a newly-developed oxidation flow reactor to study SOA formation from wood burning, we find that IVOCs can contribute ～70% of the formed SOA, i.e.>2 times more than VOCs. This previously missing SOA fraction is interpreted to be due to the high wall losses of semi-volatile oxidation products of IVOCs in smog chambers. The finding in this study reveals that SOA production from biomass burning is much higher than previously thought, and highlights the urgent need for more research on the IVOCs from biomass burning and potentially other emission sources.

关键词： atmospheric chemistry biomass burning secondary organic aerosol intermediate volatility organic compounds

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Typhoon-and pollution-driven enhancement of reactive bromine in the mid-latitude marine boundary layer

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National Science Review 2024年第4期11卷 93-101页

作者： Shanshan Wang Qinyi Li Ruifeng Zhang Anoop Sharad Mahajan Swaleha Inamdar Nuria Benavent Sanbao Zhang Ruibin Xue Jian Zhu Chenji Jin Yan Zhang Xiao Fu Alba Badia Rafael P.Fernandez Carlos A.Cuevas Tao Wang Bin Zhou Alfonso Saiz-Lopez Shanghai Key Laboratory of atmospheric Particle Pollution and Prevention (LAP3) Department of Environmental Science and Engineering Fudan University Institute of Eco-Chongming(IEC) Department of atmospheric chemistry and Climate Institute of Physical Chemistry Blas CabreraCSIC Department of Civil and Environmental Engineering The Hong Kong Polytechnic University Environment Research Institute Shandong University Centre for Climate Change Research Indian Institute of Tropical MeteorologyMinistry of Earth Sciences Department of chemistry University of Colorado Boulder Institute of Environment and Ecology Tsinghua Shenzhen International Graduate SchoolTsinghua University Sostenipra Research Group Institute of Environmental Science and Technology(ICTA)Universitat Autonoma de Barcelona(UAB) Institute for Interdisciplinary Science (ICB) National Research Council (CONICET)

Tropospheric reactive bromine is important for atmospheric chemistry,regional air pollution,and global *** studies have reported measurements of atmospheric reactive bromine species in different environments,and proposed their main sources,***-salt aerosol（SSA）,oceanic biogenic activity,polar snow/ice,and *** and other strong cyclonic activities（***） induce abrupt changes in different earth system processes,causing widespread destructive ***,the role of typhoons in regulating reactive bromine abundance and sources remains ***,we report field observations of bromine oxide（BrO）,a critical indicator of reactive bromine,on the Huaniao Island（HNI）in the East China Sea in July *** observed high levels of BrO below 500 m with a daytime average of9.7±4.2 pptv and a peak value of ～26 pptv under the influence of a *** field measurements,supported by model simulations,suggest that the typhoon-induced drastic increase in wind speed amplifies the emission of SSA,significantly enhancing the activation of reactive bromine from SSA *** also detected enhanced BrO mixing ratios under high NOxconditions（ppbv level） suggesting a potential pollution-induced mechanism of bromine release from *** elevated levels of atmospheric bromine noticeably increase ozone destruction by as much as ～40% across the East China *** the high frequency of cyclonic activity in the northern hemisphere,reactive bromine chemistry is expected to play a more important role than previously thought in affecting coastal air quality and atmospheric oxidation *** suggest that models need to consider the hitherto overlooked typhoon-and pollution-mediated increase in reactive bromine levels when assessing the synergic effects of cyclonic activities on the earth system.

关键词： reactive bromine atmospheric chemistry marine boundary layer atmospheric oxidation capacity marine emission

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Exploring atmospheric free-radical chemistry in China:the self-cleansing capacity and the formation of secondary air pollution

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National Science Review 2019年第3期6卷 579-594页

作者： Keding Lu Song Guo Zhaofeng Tan Haichao Wang Dongjie Shang Yuhan Liu Xin Li Zhijun Wu Min Hu Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University CAS Center for Excellence in Regional atmospheric Environment Chinese Academy of Sciences

Since 1971, it has been known that the atmospheric free radicals play a pivotal role in maintaining the oxidizing power of the troposphere. The existence of the oxidizing power is an important feature of the troposphere to remove primary air pollutants emitted from human beings as well as those from the biosphere. Nevertheless, serious secondary air-pollution incidents can take place due to fast oxidation of the primary pollutants. Elucidating the atmospheric free-radical chemistry is a demanding task in the field of atmospheric chemistry worldwide, which includes two kinds of work: first, the setup of reliable radical detection systems; second, integrated field studies that enable closure studies on the sources and sinks of targeted radicals such as OH and NO. In this review, we try to review the Chinese efforts to explore the atmospheric free-radical chemistry in such chemical complex environments and the possible link of this fast gas-phase oxidation with the fast formation of secondary air pollution in the city-cluster areas in China.

关键词： atmospheric chemistry free radicals new particle formations OH NO3

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Review of technologies and their applications for the speciated detection of RO2 radicals

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Journal of Environmental Sciences 2023年第1期123卷 487-499页

作者： Yue Gao Keding Lu Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control State Environmental Protection Key Laboratory of Atmospheric Ozone Pollution ControlCollege of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China

Peroxy radicals(RO_(2)),which are formed during the oxidation of volatile organic compounds,play an important role in atmospheric oxidation ***,the measurement of RO_(2),especially distinct species of RO_(2)radicals,is important and greatly helps the exploration of atmospheric chemistry *** the speciated detection of RO_(2)radicals remains challenging,various methods have been developed to study them in *** methods can be divided into spectroscopy and mass spectrometry *** spectroscopy methods contain laser-induced fluorescence(LIF),UV-absorption spectroscopy,cavity ring-down spectroscopy(CRDS)and matrix isolation and electron spin resonance(MIESR).The mass spectrometry methods contain chemical ionization atmospheric pressure interface time-of-flight mass spectrometry(CI-APi-TOF),chemical ionization mass spectrometry(CIMS),CI-Orbitrap-MS and the third-generation proton transfer reaction-time-of-flight mass spectrometer(PTR3).This article reviews technologies for the speciated detection of RO_(2)radicals and the applications of these *** addition,a comparison of these techniques and the reaction mechanisms of some key species are ***,possible gaps are proposed that could be filled by future research into speciated RO_(2)radicals.

关键词： Speciated RO_(2)radicals atmospheric chemistry Reaction mechanisms Mass spectrometry

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Anthropogenic emission inventories in China:a review

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National Science Review 2017年第6期4卷 834-866页

作者： Meng Li Huan Liu Guannan Geng Chaopeng Hong Fei Liu Yu Song Dan Tong Bo Zheng Hongyang Cui Hanyang Man Qiang Zhang Kebin He Ministry of Education Key Laboratory for Earth System Modeling Department for Earth System Science Tsinghua University now at Max-Planck Institute for chemistry State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University StateKey Joint Laboratory of Environmental Simulation and Pollution Control Department of Environmental SciencePeking University

The development of reliable anthropogenic emission inventories is essential for both understanding the sources of air pollution and designing effective air-pollution-control measures in China. However, it is challenging to quantify emissions in China accurately, given the variety of contributing sources, the complexity of the technology mix and the lack of reliable measurements. Over the last two decades,tremendous efforts have been made to improve the accuracy of emission inventories, and significant improvements have been realized. More reliable statistics and survey-based data have been used to reduce the uncertainties in activity rates and technology distributions. Local emission factors and source profiles covering various sources have been measured and reported. Based on these local databases, improved emission inventory models have been developed for power plants, large industrial plants and the residential,transportation and agricultural sectors. In this paper, we review the progress that has been made in developing inventories of anthropogenic emissions in China. We first highlight the major updates that have been made to emission inventory models and the underlying data by source category. We then summarize the sector-based estimates of emissions of different species contained in current inventories. The progress that has been made in the development of model-ready emissions is also presented. Finally, we suggest future directions for further improving the accuracy of emission inventories in China.

关键词： emission inventory atmospheric chemistry China chemical transport model air pollution

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Mechanisms and Kinetics of Reaction CHCIBr＋NO2

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Chemical Research in Chinese Universities 2015年第6期31卷 1018-1022页

作者： YANG Lei LIU Yuyu DUAN Xuemei Institute of Theoretical chemistry Jilin University Changehun 130021 P. R. China Center for Molecular Systems and Organic Devices Key Laboratory forOrganic Electronics & Information Displays and Institute of Advanced MaterialsNanjing University of Posts and Telecommunications Nanjing 210023 R R. China

The reaction CHClBr＋NO2 was investigated via quantum chemical methods and kinetic calculations. The reaction mechanism on the singlet potential energy surface（PES） was considered by B3LYP method, and the energies were calculated at the CCSD（T） and CASPT2 levels of theory. The rate constants and the ratios of products were obtained by utilizing VTST and RRKM methods over wide temperature and pressure ranges. Our results indicate that carbon-to-nitrogen approach via a barrierless process is preferred in the initial association of CHClBr and NO2. The dominant product is BrNO＋CHCIO（PI）, which agrees well with the experimental observation. P2（ClNO＋CHBrO） and P3（HNO＋CBrClO） may also have minor contributions to the reaction. The calculated overall rate constants are independent of pressure and consistent with the experimental data, which can be fitted with the following equation over the temperature range of 200--1500 K： k（T）=2.31 × 10^-15T^0.99exp（771/T）. Compared with reaction CH2Br＋NO2, reaction CHCIBr＋NO2 has decreased the overall rate constants.

关键词： Transition-state theory Master equation simulation atmospheric chemistry Combustion chemistry Carbon-centered free radical

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Theoretical Study on Impact of Single Water Molecule on OH＋O3 Reaction

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Chinese Journal of Chemical Physics 2011年第4期24卷 419-424,I0003页

作者：龙波张为俊隆正文贵州民族学院计算机与信息工程学院贵阳550025 贵州大学物理系贵阳550025 中国科学院安徽光学精密机械研究所环境光学实验室合肥230031

Quantum chemical calculations are performed to study the reactions of OH and ozone with- out and with water to estimate whether the single water molecule can decrease the energy barrier of the OH radical reaction with ozone. The calculated results demonstrate that the single water molecule can reduce the activated barrier of the naked OH＋Oa reaction with the value of about 4.18 kJ/mol. In addition, the transition state theory is carried out to determine whether the single water molecule could enhance the rate constant of the OH＋O3 reaction. The computed kinetic data indicate that the rate of the ozone reaction with the formed complexes between OH and water is much slower than that of the OH＋O3 reaction, whereas the rate constant of OH reaction with the formed H20---Oa complex is 2 times greater than that of the naked OH radical with ozone reaction. However, these processes in the atmosphere are not important because the reactions can not compete well with the naked reaction of OH with ozone under atmospheric condition.

关键词： Ozone OH H20 atmospheric chemistry Quantum chemical calculation

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