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Underestimated benefits of NO_(x) control in reducing SNA and O_(3) based on missing heterogeneous HONO sources

Frontiers of Environmental Science & Engineering 2024年第3期18卷 57-67页

作者： Shuping Zhang Haotian Zheng Jun Liu Yao Shi Tianzeng Chen Chaoyang Xue Fenfen Zhang Yueqi Jiang Xiangping Zhang Shovan Kumar Sahu biwu chu Jia Xing State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China China Academy of Civil Aviation Science and Technology Beijing 100028China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Yellow River Institute of Hydraulic Research Zhengzhou 450003China Centre for Climate Research Singapore Meteorological Service SingaporeSingapore 537054Singapore

Substantial NO_(x) emission mitigation is crucial for the synergistic reduction of particulate matter and ozone(O_(3))pollution in *** traditional air quality model does not consider heterogeneous HONO chemistry,leading to uncertainties in estimating the benefits of NO_(x) *** studies have shown that the parameterization of heterogeneous HONO formation increases both the simulated value of sulfate–nitrate–ammonium(SNA)and that of O_(3),thus adding the heterogeneous reactions of HONO into air quality models inevitably leads to changes in the estimated benefits of NO_(x) *** we investigated the changes in SNA and O_(3)concentrations from NO_(x) emission reduction before and after adding heterogeneous HONO reactions in the Community Multi-Scale Air Quality(CMAQ)*** heterogeneous HONO reactions in the simulation improved the benefits of NO_(x) reduction in terms of SNA control in *** 80%NO_(x) reduction,the reduction in SNA increased from 36.9%without considering heterogeneous HONO reactions to 42.8%with heterogeneous HONO *** reduction in the maximum daily 8h average(MDA8)O_(3)in summer caused by NO_(x) reduction increased slightly from 4.7%to 5.2%after adding heterogeneous HONO *** results in this study highlight the enhanced effectiveness of NO_(x) controls for the reduction of SNA and O_(3)after considering heterogeneous HONO formation in a complex chemical ambient,demonstrating the importance of NO_(x) controls in reducing PM2.5 and O_(3)pollution in China.

关键词： Heterogeneous HONO NO_(x) reduction PM_(2.5) O_(3)

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

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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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“环境催化城市”:概念提出和研究展望

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化学进展 2024年第4期36卷 466-470页

作者：马金珠楚碧武马庆鑫何广智刘倩王书肖贺克斌赵进才贺泓中国科学院生态环境研究中心北京100085 中国科学院化学研究所北京100080 清华大学北京100084 中国科学院大学北京101413 中国科学院城市环境研究所厦门361021

大气污染是城市环境质量改善面临的重大挑战。城市化过程既是造成城市大气高度复合污染的重要原因,也为城市自净化大气污染物提供了可人为强化的条件。“环境催化城市”是指将城市中的建筑物内外、硬化地面等表面涂覆催化材料,在自然界... 详细信息

大气污染是城市环境质量改善面临的重大挑战。城市化过程既是造成城市大气高度复合污染的重要原因,也为城市自净化大气污染物提供了可人为强化的条件。“环境催化城市”是指将城市中的建筑物内外、硬化地面等表面涂覆催化材料,在自然界的光、热等条件下实现环境中低浓度气态污染物自发催化净化的城市。构建“环境催化城市”对低碳控制大气复合污染,持续改善室内外环境空气质量,规划建设“自净城市”意义重大。本文提出了“环境催化城市”概念,并对如何完善和发展“环境催化城市”理论和实践进行了展望。

关键词：环境催化城市霾化学环境容量臭氧催化分解自净城市

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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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Coordinated Control of Fine-Particle and Ozone Pollution by the Substantial Reduction of Nitrogen Oxides

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Engineering 2022年第8期8卷 13-16页

作者： biwu chu Yan Ding Xiang Gao Junhua Li Tingyu Zhu Yunbo Yu 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 Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China University of the Chinese Academy of Sciences Beijing 100049China Chinese Research Academy of Environmental Sciences Beijing 100012China State Environmental Protection Engineering Center for Coal-Fired Air Pollution Control Zhejiang UniversityHangzhou 310027China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

*** In recent years,the air quality in China has improved *** many cities,however,the concentration of fine particulate matter(PM_(2.5))remains higher than the secondary-level national ambient air quality standard(NAAQS level-2,35μg·m^(-3),GB3095-2012[1])and much higher than the first-level NAAQS(15μg·m^(-3),GB3095-2012[1])and the World Health Organization(WHO)air quality guidelines(5μg·m^(-3)).

关键词： Pollution Ozone ambient

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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 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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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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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：城市地区浓度增加北京市区郊区比较测量污染亚硝酸非均相反应

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