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Mechanism for the promotional formation of NH_(4)^(+) by SO_(2) on different mineral dust surfaces

Particuology 2023年第4期75卷 109-118页

作者： Hao Li Qingxin Ma biwu chu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing100085China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen361021China Institute of Atmospheric Physics Chinese Academy of SciencesBeijing100029China

Ammonium is an important atmospheric particulate component that dictates many environmental *** promotion of the heterogeneous conversion of NH_(3) to NH_(4)^(+) by SO_(2) on different mineral dust surfaces displays remarkable discrepancies,especially on MgO and α-Fe2O3 surfaces,however,the underlying mechanisms are not well ***,using periodic density functional theory(DFT)calculation and Born-Oppenheimer molecular dynamics(BOMD)simulation,we explored the hetero-geneous adsorption of NH_(3) on MgO(110)and α--Fe2O3(001)surfaces in the presence and absence of SO_(2).The results show that on MgO(110)surface,hydrogen-bonding interactions of NH_(3) on both adsorbed hydroxyl or bisulfite/bisulfate sites are observed no matter whether SO_(2) is present or ***,on theα-Fe2O3(001)surface,significant conversion of NH_(3) to NH_(4)^(+)occurs with the coexistence of SO_(2),which is due to the hydrogen transfer reaction from surface HSO4 to N in NH_(3).The fundamental reason may be that the stronger electron affinity of Fe3+than Mg2+results in adsorbed bisulfate and/or bisulfite with greater acidity on α-Fe2O3 surface than MgO *** results give a molecular-level explanation for the heterogeneous conversion of NH_(3) to NH_(4)^(+)on different mineral dust surfaces under complex air pollution *** the fact that ammonium is abundant in secondary particulates,this work would help in understanding the rapid conversion of ammonia to ammonium and in developing classification governance policies for the key precursor pollutants in China.

关键词： Mineral dust Heterogeneous reaction Theoretical calculation Ammonium SO_(2)

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Effects of seed particles Al2O3, Al2（SO4）3 and H2SO4 on secondary organic aerosol

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Frontiers of Environmental Science & Engineering 2017年第4期11卷 161-169页

作者： Xiao Zhang biwu chu Junhua Li Chaozhi Zhang School of Environmental Science and Engineering Nanjing University of Information Science & Technology Nanjing 210044 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China

Seed particles Al2O3, Al2（SO4）3 and H2SO4 were selected to investigate their effects on secondary aerosol （SA） formation in toluene/NOx photooxidation under sulfur dioxide （SO2） and ammonia （NH3）. Effect of seed particles on SA formation was related to their acid-base properties and the presence of acid or alkaline gases. Under NH3-poor condition, SA formation increased with increasing SO2 concentration due to the acid-catalyzing effect of the oxidation products of SO2 （i.e. H2SO4）, The enhancing effect of SO2 became unobvious under NH3-rieh condition, because NH3 would eliminate the acid-catalyzing effect by neutralizing the acid products. Acidic seeds H2SO4 accelerated SA formation under either SO2 or NH3 condition. Weak acidic Al2（SO4）3 seeds didn＇t affect obviously on SA formation. The inhibiting effect of amphoteric seeds Al2O3 on SA formation was related to the presence of SO2 / NH3 due to their acid-base property. Under NH3-poor condition, the inhibiting effect of Al2O3 on SA formation decreased with increasing concentration of SO2, while under NH3-rich condition, the inhibiting effect wasn＇t remarkable.

关键词： Seed particle Secondary aerosol Sulfur dioxide Ammonia Acid-catalyzing effect

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Homogeneous and heterogeneous photolysis of nitrate in the atmosphere:state of the science,current research needs,and future prospects

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Frontiers of Environmental Science & Engineering 2023年第4期17卷 109-126页

作者： Yiqun Cao Qingxin Ma biwu chu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China College of Resources and Environment University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

Nitrate is an important component of atmospheric particulate matter and affects air quality,climate,human health,and the *** was previously considered a permanent sink for nitrogen oxides(NO_(x)).However,this viewpoint has been challenged in recent years because growing research evidence has shown the transformation of nitrate into NO_(x)(i.e.,renoxification).The photolysis of nitrate/HNO3,especially in the particulate phase or adsorbed on particles,can be a significant renoxification process in the *** formation and photolysis of nitrate in aerosol not only change the diurnal variation of NO_(x),but also provide long-distance transport of NO_(x)in the form of nitrate,which affects local and regional atmospheric chemistry and air *** review summarizes recent advances in the fundamental understanding of the photolysis of nitrate/HNO3 under various atmospheric conditions,with a focus on mechanisms and key factors affecting the *** atmospheric implications are discussed and future research is recommended.

关键词： Nitrate Photolysis Renoxification Aerosol

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Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NOx photooxidation

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Frontiers of Environmental Science & Engineering 2013年第1期7卷 1-9页

作者： biwu chu Jiming HAO Junhua LI Hideto TAKEKAWA Kun WANG Jingkun JIANG State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China Toyota Central Research and Development Laboratory Nagakute Aichi 480-1192 Japan

Aerosol phase reactions play a very important role on secondary organic aerosol (SOA) formation, and metal-containing aerosols are important components in the atmosphere. In this study, we tested the effects of two transition metal sulfate salts, manganese sulfate (MnSO ) and zinc sulfate (ZnSO ), on the photochemical reactions of a toluene/NO photooxidation system in a 2 m smog chamber. By comparing photochemical reaction products of experiments with and without transition metal sulfate seed aerosols, we evaluated the effects of transition metal sulfate seed aerosols on toluene consumption, NO conversion and the formation of ozone and SOA. MnSO and ZnSO seed aerosols were found to have similar effects on photochemical reactions, both enhance the SOA production, while showing negligible effects on the gas phase compounds. These observations are consistent when varying metal sulfate aerosol concentrations. This is attributed to the catalytic effects of MnSO and ZnSO seed aerosols which may enhance the formation of condensable semivolatile compounds. Their subsequent partitioning into the aerosol phase leads to the observed SOA formation enhancement.

关键词： manganese sulfate zinc sulfate seed aerosols toluene photooxidation secondary organic aerosol

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Distinct potential aerosol masses under different scenarios of transport at a suburban site of Beijing

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Journal of Environmental Sciences 2016年第1期28卷 52-61页

作者： biwu chu Yongchun Liu Qingxin Ma Jinzhu Ma Hong He Gang Wang Shuiyuan Cheng Xinming Wang State Key Joint Laboratory of Environmental Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of Sciences Key Laboratory of Beijing on Regional Air Pollution Control Beijing University of Technology State Key Laboratory of Organic Geochemistry Guangzhou Institute of Geochemistry Chinese Academy of Sciences

In order to evaluate the secondary aerosol formation potential at a suburban site of Beijing,in situ perturbation experiments in a potential aerosol mass（PAM） reactor were carried out in the winter of *** variations of secondary aerosol formation as a function of time,OH exposure,and the concentrations of gas phase pollutants and particles were reported in this *** periods with distinct secondary aerosol formation potentials,marked as Period Ⅰ and Period Ⅱ,were identified during the *** Period Ⅰ,the secondary aerosol formation potential was high,and correlated well to the air pollutants,i.e.,SO2,NO2,and *** maximal secondary aerosol formation was observed with an aging time equivalent to about 3 days of atmospheric *** period Ⅱ,the secondary aerosol formation potential was low,with no obvious correlation with the air ***,the aerosol mass decreased,instead of showing a peak,with increasing aging *** trajectory analysis during the two periods confirmed that the air mass in Period Ⅰwas mainly from local sources,while it was attributed mostly to long distance transport in Period Ⅱ.The air lost its reactivity during the long transport and the particles became highly aged,resulting in a low secondary aerosol formation *** experimental results indicated that the in situ measurement of the secondary aerosol formation potential could provide important information for evaluating the contributions of local emission and long distance transport to the aerosol pollution.

关键词： Potential aerosol mass Local emission Long distance transport Aging In situ perturbation experiments

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Atmospheric heterogeneous reactions on soot:A review

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Fundamental Research 2023年第4期3卷 579-591页

作者： Yuan Liu Guangzhi He biwu chu Qingxin Ma Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China

Soot particles,composed of elemental carbon and organic compounds,have attracted widespread attention in recent years due to their significant impacts on climate,the environment and human *** has been found to be chemically and physically active in atmospheric aging processes,which leads to alterations in its composition,morphology,hygroscopicity and optical properties and thus changes its environmental and health *** heterogeneous reactions on soot also have a significant impact on the transformation of gaseous pollutants into secondary ***,the interactions between soot and atmospheric substances have been widely investigated to better understand the environmental behaviors of *** this review,we systematically summarize the progress and developments in the heterogeneous chemistry on soot over the past_(3)0 *** trace constituents such as NO_(2),O_(3),SO_(2),N_(2)O_(5),HNO_(3),H_(2)SO_(4),OH radical,HO_(2)radical,peroxyacetyl nitrate etc.,are presented in detail from the aspect of their heterogeneous reactions on *** possible mechanisms and the effects of environmental conditions on these heterogeneous reactions are also ***,the impacts of the heterogeneous reactions of soot on the atmospheric environment are discussed,and some aspects of soot-related research which require further investigation are proposed as well.

关键词： Soot NO_(2) SO_(2) O_(3) Heterogeneous reactions

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Comparisons of measured nitrous acid(HONO) concentrations in a pollution period at urban and suburban Beijing, in autumn of 2014

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Science China Chemistry 2015年第9期58卷 1393-1402页

作者： Shengrui Tong Siqi Hou Ying Zhang biwu chu Yongchun Liu Hong He Pusheng Zhao Maofa Ge State Key Laboratory for Structural Chemistry of Unstable and Stable Species Beijing National Laboratory for Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Institute of Urban Meteorology China Meteorological Administration

To study the HONO formation mechanisms during a pollution period, a continuous measurement was performed in both urban and suburban aeras of Beijing. During this period, the PM2.5 concentrations increased to 201 and 137 ?g/m3 in urban and suburban areas, respectively. The concentrations of HONO, CO, SO2, O3, NO, NO2, NOx were 1.45 ppbv, 0.61 ppmv, 8.7 ppbv, 4.3 ppbv, 44.4 ppbv, 37.4 ppbv, 79.4 ppbv and 0.72 ppbv, 1.00 ppmv, 1.2 ppbv, 7.9 ppbv, 3.7 ppbv, 8.2 ppbv, 11.9 ppbv, in urban and suburban areas, respectively. To compare possible pathways of HONO formation in both sites, the contributions of direct emissions, heterogeneous formations, and homogeneous productions were studied. HONO/NO2 ratios in the two sites indicated that heterogeneous reactions of NO2 were more efficient in suburban areas. And in both urban and suburban areas, the increase of PM2.5 concentrations and RH would promote the conversion efficiency in RH that ranged from 0% to 85%. However, when RH was above 85%, the HONO formation slowed down. Moreover, the study of direct emissions and homogeneous reactions showed that they contributed to a majority of HONO increase in urban areas than the 20% contributions in suburban areas. It implied that the high NOx concentrations and NO concentrations in urban areas or in pollution periods would make direct emissions and homogeneous reactions become dominant in HONO formations.

关键词： nitrous acid pollution urban suburban comparison

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Effect of aluminium dust on secondary organic aerosol formation in m-xylene/NO_x photo-oxidation

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Science China Earth Sciences 2015年第2期58卷 245-254页

作者： LIU Chang MA QingXin chu biwu LIU Yongchun HE Hong ZHANG XiaoYe LI JunHua HAO JiMing Chinese Academy of Meteorological Sciences Research Center for Eco-Environmental Sciences Chinese Academy of Sciences School of Environment Tsinghua University

As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds(boehmite and alumina) on SOA yield and aerosol size in m-xylene/NOx photo-oxidation were investigated in a 2 m3 smog chamber at 30°C and 50% relative humidity. Compared to the seed-free system, the presence of aluminium seeds resulted in an increase in the SOA yield, and also enhanced the O3 concentration in the chamber. The photolysis of O3 is a major source of OH radical, which is the most important oxidant of m-xylene. The increase in O3 concentration could result in the generation of more OH radicals, and finally contribute to the SOA formation. Seed particles influence the SOA size mainly by acting as condensation nuclei. Semi-volatile organic compounds(SVOCs) were condensed onto these nuclei, resulting in the increase in SOA size. However, when aluminium seeds with high concentrations were introduced into the system, SVOCs that had been condensed onto each particle were dispersed by these seeds, leading to the reduction in aerosol size.

关键词： aerosol xylene chamber aluminium anthropogenic volatile nuclei humidity dispersed oxidant

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Differences of the oxidation process and secondary organic aerosol formation at low and high precursor concentrations

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Journal of Environmental Sciences 2019年第5期31卷 256-263页

作者： Tianzeng Chen Yongchun Liu biwu chu Changgeng Liu Jun Liu Yanli Ge Qingxin Ma Jinzhu Ma Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences University of Chinese Academy of Sciences Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences

Current atmospheric quality models usually underestimate the level of ambient secondary organic aerosol(SOA), one of the possible reasons is that the precursors at different concentrations may undergo different oxidation processes and further affect SOA formation. Therefore, there is a need to perform more chamber studies to disclose the influence. In this work, SOA formation over a wide range of initial precursor concentrations(tens of ppb to hundreds of ppb levels) was investigated in a 30 m3 indoor smog chamber,and mainly through the analysis of multiple generations of VOCs detected from HR-To FPTRMS to expound the difference in the oxidation process between low and high precursor concentrations. Compared to high initial concentrations, gas-phase intermediates formed at low concentrations had a higher intensity by about one order of magnitude, and the lowvolatility compounds also had a higher formation potential due to the competition between semi-volatile intermediates and precursors with oxidants. In addition, the formed SOA was more oxidized with higher f44 value(0.14 ± 0.02) and more relevant to real atmosphere than that formed at high concentrations. This work should help to deeply understand SOA formation and improve the performance of air quality models for SOA simulation.

关键词： Secondary organic aerosol Aromatic hydrocarbons Aerosol mass spectrometer Low-volatility compounds Oxidation processes

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Hygroscopicity of particles generated from photooxidation of α-pinene under diferent oxidation conditions in the presence of sulfate seed aerosols

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Journal of Environmental Sciences 2014年第1期26卷 129-139页

作者： biwu chu Kun Wang Hideto Takekawa Junhua Li Wei Zhou Jingkun Jiang Qinxing Ma Hong He Jiming Hao State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Research Center for Eco-Environmental Science Chinese Academy of Sciences Toyota Central Research and Development Laboratory

Smog chamber experiments were conducted to investigate the hygroscopicity of particles generated from photooxidation of α-pinene/NOx with different sulfate seed aerosols or oxidation conditions. Hygroscopicity of particles was measured by a tandem differential mobility analyzer （TDMA） in terms of hygroscopic growth factor （Gf）, with a relative humidity of 85%. With sulfate seed aerosols present, Gf of the aerosols decreased very fast before notable secondary organic aerosols （SOA） formation was observed, indicating a heterogeneous process between inorganic seeds and organic products might take place as soon as oxidation begins, rather than only happening after gas-aerosol partition of organic products starts. The final SOA-coated sulfate particles had similar or lower Gf than seed-free SOA. The hygroscopicity of the final particles was not dependent on the thickness but on the hygroscopicity properties of the SOA, which were influenced by the initial sulfate seed particles. In the two designed aging processes, Gf of the particles increased more significantly with introduction of OH radical than with ozone. However, the hygroscopicity of SOA was very low even after a long time of aging, implying that either SOA aging in the chamber was very slow or the Gf of SOA did not change significantly in aging. Using an aerosol composition speciation monitor （ACSM） and matrix factorization （PMF） method, two factors for the components of SOA were identified, but the correlation between SOA hygroscopicity and the proportion of the more highly oxidized factor could be either positive or negative depending on the speciation of seed aerosols present.

关键词： hygroscopicity sulfate seed aerosols secondary organic aerosol α-pinene photooxidation aging

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