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Progress in quantitative research on the relationship between atmospheric oxidation and air quality

Journal of environmental Sciences 2023年第1期123卷 350-366页

作者： Yuesi Wang Xin Jin 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 State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China 3 State Key Joint Laboratory or Environmental Simul ation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Key Lab of Geophysical Information System of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 200241China Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Department of Environmental Science and EngineeringFudan UniversityShanghai 201203China Key Lab of Aerosol Chemistry and Physics State Key Laboratory of Loess and Quaternary GeologyInstitute of Earth EnvironmentChinese Academy of SciencesXi’an 710061China Institute of Atmospheric Composition and Environmental Meteorology Chinese Academy of Meteorological SciencesBeijing 100081China Key Lab of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China

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 *** 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 *** paper will give a brief review of these ***,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 *** addition,the detection of ground or vertical profiles for atmospheric OH·,HO_(2)·,NO_(3)·radicals and reservoir molecules can now be obtained with domestic instruments in diverse ***,laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O_(3)and NO_(2),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 ***,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 *** numerical simulations of AOIe and AOIp were performed,and regional coordination of AOC was *** optimized plan for controlling O_(3)and PM2.5was analyzed by scenario simulation.

关键词： Atmospheric oxidizing capacity(AOC) Quantitative index Free radicals Observation and modeling Air quality

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Formaldehyde oxidation on Pd/USY catalysts at room temperature: The effect of acid pretreatment on supports

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Journal of environmental Sciences 2023年第3期125卷 811-822页

作者： Xiaofeng Liu Chunying Wang Yumin Chen Qi Qin Yaobin Li Hong He Center for Excellence in Regional Atmospheric Environment Key Laboratory of Urban Pollutant ConversionChinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Chinese Academy of SciencesNingbo Urban Environment Observation and Research Station-NUEORSNingbo 315800China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing 100085China Xiamen Key Laboratory of Materials for Gaseous Pollutant Control Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

The complete catalytic oxidation of formaldehyde (HCHO) to CO_(2)and H_(2)O at room temperature is a green route for indoor HCHO *** is an excellent carrier material for HCHO oxidation due to its large surface area,intricate pores and high adsorption ***,the zeolite-supported noble metal catalysts have currently shown relatively low activity especially at room *** this work,we present a facile acid treatment strategy for zeolite catalysts to improve the hydroxyl concentration and further enhance their catalytic activity for HCHO *** tests illustrated that HCHO could be completely oxidized to CO_(2)and H_(2)O at a nearly 100%conversion rate with a weight hourly space velocity (WHSV) of 150,000 mL/(g·hr) at 25℃,when the support of Pd/USY catalysts was pretreated by hydrochloric acid with a concentration of 0.20 mol/*** characterization results revealed that the active hydroxyl groups originated from the dealumination in the acid treatment play a key role in the HCHO oxidation *** deduced reaction mechanism suggests that bridging hydroxyl groups may oxidize HCHO to dioxymethylene(DOM) species and terminal hydroxyl groups are responsible for the transformation of DOM groups to formate (HCOO) species.

关键词： Formaldehyde oxidation USY zeolite Acid treatment Hydroxyl groups

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Global methyl halide emissions from biomass burning during 2003-2021

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environmental Science and Ecotechnology 2023年第2期14卷 79-86页

作者： Xiaoyi Hu Di Chen Liting Hu Bowei Li Xinhe Li Xuekun Fang College of Environmental&Resource Sciences Zhejiang UniversityHangzhouZhejiang310058PR China State Key Joint Laboratory for Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing100871PR China Center for Global Change Science Massachusetts Institute of TechnologyCambridgeMA02139USA

Methyl halides(CH3Cl,CH3Br,and CH3I)are ozone-depleting *** burning(BB)is an important source of methyl *** temporal variations and global spatial distribution of BB methyl halide emissions are ***,global methyl halide emissions from BB during 2003e2021 were estimated based on satellite data.A significant decreasing trend(p<0.01)in global methyl halide emissions from BB was found between 2003 and 2021,with CH3Cl emissions decreasing from 302 to 220 Gg yr^(-1),CH3Br emissions decreasing from 16.5 to 11.7 Gg yr^(-1),and CH3I emissions decreasing from 8.9 to 6.1 Gg yr^(-1).From a latitudinal perspective,the northern high-latitude region(60e90N)was the only latitude zone with significant increases in BB methyl halide emissions(p<0.01).Based on an analysis of the drivers of BB methyl halide emissions,emissions from cropland,grassland,and shrubland fires were more correlated with the burned area,while BB emissions from forest fires were more correlated with the emissions per unit burned *** non-BB emissions of CH3Cl increased from 4749 Gg yr^(-1)in 2003 to 4882 Gg yr^(-1)in 2020,while those of CH3Br decreased from 136 Gg yr^(-1)in 2003 to 118 Gg yr^(-1)in 2020(global total CH3I emissions are not available).The finding indicates that global CH3Cl and CH3Br emissions from sources besides BB increased and decreased during *** on our findings,not only searching for unknown sources is important,but also re-evaluating known sources is necessary for addressing methyl halide emissions.

关键词： Methyl halides Biomass burning Emission inventory Global budget Ozone depletion

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A superior catalyst for ozone decomposition: NiFe layered double hydroxide

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Journal of environmental Sciences 2023年第12期134卷 2-10页

作者： Zhisheng Wang Yingfa Chen Xiaotong Li Jinzhu Ma Guangzhi He 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 Chinese Academy of Sciences Beijing 100049China

Ground-level ozone is harmful to human beings and ecosystems,while room-temperature catalytic decomposition is the most effective technology for ozone ***,solving the deactivation of existing metal oxide catalysts was caused by oxygen-containing intermediates is ***,we successfully prepared a two-dimensional NiFe layered double hydroxide (NiFe-LDH) catalyst via a facile co-precipitation method,which exhibited stable and highly efficient performance of ozone decomposition under harsh operating conditions (high space velocity and humidity).The NiFe-LDH catalyst with Ni/Fe=3and crystallization time over 5 hr (named Ni3Fe-5) exhibited the best catalytic performance,which was well beyond that of most existing manganese-based oxide ***,under relative humidity of 65%and space velocity of 840 L/(g·hr),Ni3Fe-5 showed ozone conversion of 89%and 76%for 40 ppmV of O3within 6 and 168 hr at room-temperature,*** demonstrated that the layered structure of NiFe-LDH played a decisive role in its outstanding catalytic performance in terms of both activity and water *** LDH catalysts fundamentally avoids the deactivation caused by the occupancy of oxygen vacancies by oxygen-containing species (H2O,O-,and O2-) in manganese-based *** study indicated the promising application potential of LDHs than manganese-based oxide catalysts in removal of gaseous ozone.

关键词： Ozone decomposition Confined catalysis Nickel-iron layered double hydroxides Co-precipitation method Two-dimensional materials

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Electrostatic removal of ultrafine carbon black with square-grooved collecting plates:Insights for capturing black carbon emitted from ships

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Journal of environmental Sciences 2024年第2期136卷 559-569页

作者： Zhicheng Wu YifanWang Lingyu Shao Hao Zhang Haobo Dai Haidong Fan Chenghang Zheng Xiang Gao State Key Lab of Clean Energy Utilization State Environmental Protection Engineering Center for Coal-Fired Air Pollution ControlZhejiang UniversityHangzhou 310027China Department of Earth and Environmental Sciences University of ManchesterOxford RoadUnited Kingdom Zhejiang Tiandi Environmental Protection Engineering Co. Ltd.Hangzhou 310012China Baima Lake Laboratory(Zhejiang Provincial Laboratory of Energy and Carbon Neutrality) Hangzhou 310000China

Ships and other mobile pollution sources emitted massive ultrafine and low-resistivity particles containing black carbon(BC),which were harmful to human health and were difficult to capture by conventional electrostatic precipitators(ESPs).In this study,nanoscale carbon black was adopted as simulated particles(SP)with similar physicochemical properties for black carbon emitted from ships(SP-BC)to investigate the feasibility of using an ESP with square-grooved collecting plates for the removal of SP-BC at low *** increased applied voltage significantly improved the total collection of SP-BC whereas may also promote the conversion of relatively larger particle size SP-BC into nano-size below *** outlet number concentration of SP-BC under 27 kV at 130℃was three times that of the *** the reduction of the flow rate could strengthen the capture of SP-BC below20 nm,and under the combined action of low flow rate and maximum applied voltage,the collection efficiency of 20-100 nm SP-BC could exceed 90%.In addition,the escape and capture characteristics of SP-BC under long-term rapping were *** square-grooved collecting plate could effectively restrain the re-entrainment of collected SP-BC generated by rapping,and the nanoscale SP-BC was trapped in the grooves after *** results could provide insights into the profound removal of massive nanoscale black carbon emissions from mobile sources.

关键词： Simulated ship black carbon Electrostatic removal Square-grooved collecting plate Long-term rapping

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Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

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Frontiers of environmental Science & Engineering 2022年第4期16卷 27-36页

作者： Qinjun Liang Yu Gao Zhigang Li Jiayi Cai Na Chu Wen Hao Yong Jiang Raymond Jianxiong Zeng Fujian Provincial Key Laboratory of Soil Environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

Microbial electrosynthesis(MES)is an emerging technology for producing chemicals,and coupling MES to anodic waste oxidation can simultaneously increase the competitiveness and allow additional functions to be *** this study,MES was used for the simultaneous removal of ammonia from synthetic urine and production of acetate from CO_(2).Using graphite anode,83.2%±5.3%ammonia removal and 28.4%±9.9%total nitrogen removal was achieved,with an energy consumption of 1.32 kWh/g N for total nitrogen removal,0.45 kWh/g N for ammonia nitrogen removal,and 0.044 kWh/g for acetate *** boron-doped diamond(BDD)anode,70.9%±12.1%ammonia removal and 51.5%±11.8%total nitrogen removal was obtained,with an energy consumption of 0.84 kWh/g N for total nitrogen removal,0.61 kWh/g N for ammonia nitrogen removal,and 0.043 kWh/g for acetate production.A difference in nitrate accumulation explained the difference of total nitrogen removal *** of ammonia and acetate across the membrane deteriorated the performance of *** results are important for the development of novel elcctricity-driven technologies for chemical production and pollution removal.

关键词： Biocathode Carbon dioxide Electrochemical oxidation Graphite anode Boron-doped diamond

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Real-Time Black Carbon Emissions from Light-Duty Passenger Vehicles Using a Portable Emissions Measurement System

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Engineering 2022年第9期16卷 73-81页

作者： Xuan Zheng Liqiang He Xiaoyi He Shaojun Zhang Yihuan Cao Jiming Hao Ye Wu College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China Center for Sustainable Systems School for Environment and SustainabilityUniversity of MichiganAnn ArborMI 48109-1041USA State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084China

Black carbon(BC)is considered the second largest anthropogenic climate forcer,but the radiative effects of BC are highly correlated with its combustion ***-road vehicles are an important source of anthropogenic ***,there are major uncertainties in the estimates of the BC emissions from on-road light-duty passenger vehicles(LDPVs),and results obtained with the portable emissions measurement system(PEMS)method are particularly *** developed a PEMS platform and evaluated the on-road BC emissions from ten in-use *** demonstrated that the BC emission factors(EFs)of gasoline direction injection(GDI)engine vehicles range from 1.10 to 1.56 ***^(-1),which are higher than the EFs of port fuel injection(PFI)engine vehicles(0.10–0.17 ***^(-1))by a factor of *** BC emissions during the cold-start phase contributed 2%–33%to the total emissions.A strong correlation(R^(2)=0.70)was observed between the relative BC EFs and average vehicle speed,indicating that traffic congestion alleviation could effectively mitigate BC ***,BC and particle number(PN)emissions were linearly correlated(R^(2)=0.90),and compared to PFI engine vehicles,the instantaneous PN-to-BC emission rates of GDI engine vehicles were less sensitive to vehicle specific power-to-velocity(VSPV)increase in all speed ranges.

关键词： Black carbon Light-duty gasoline vehicles Portable emissions measurement system Real-time emissions

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Tuning SMSI to stabilize metallic Pd species:A case study on Pd/TiO_(2) for HCHO oxidation

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Chinese Chemical Letters 2024年第3期35卷 162-166页

作者： Chunying Wang Xiaofeng Liu Jingyi Wang Yaobin Li Shaohua Xie Fudong Liu Changbin Zhang Yuming Zheng Wenpo Shan Hong He Center for Excellence in Regional Atmospheric Environment Key Laboratory of Urban Pollutant ConversionInstitute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research StationChinese Academy of SciencesNingbo 315800China Department of Civil Environmentaland Construction Engineering(CECE)Catalysis Cluster for Renewable Energy and Chemical Transformations(REACT)Nano Science Technology Center(NSTC)University of Central FloridaOrlandoFL 32816USA State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing 100085China

Pretreatment of the carrier for supported catalysts can effectively improve the strong metal-support interaction(SMSI)and increase the dispersion of precious metals,which are critical to many important catalytic *** this work,we tuned SMSI on Pd/TiO_(2)catalysts through inducing surface defects of TiO_(2)by pretreated with different atmospheres(H_(2)/N_(2),N_(2),O_(2)/N_(2))at the high temperature(800℃).Multiple characterization results illustrated that surface defects anchored Pd species and thus enhanced their *** reduction,Ti^(3+)species formed and transferred onto the metallic Pd species and then induced SMSI,which effectively stabilize Pd species in the metallic *** stronger MSI,the more stability of Pd *** a case,Pd/TiO_(2)–800H_(2),with strongest MSI,displayed the best HCHO oxidation performance at low temperature(10℃).

关键词： Pd/TiO_(2) Surface defects SMSI Formaldehyde Stability of Pd species

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Thallium spill shifts the structural and functional characteristics of viral communities with different lifestyles in river sediments

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Science of the Total Environment 2024年 947卷 174531页

作者： Zhu, Ying Yan, Shuang Chen, Xiuli Li, Yangyang Xie, Shuguang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing100871 China

Thallium (Tl), a highly toxic heavy metal, can affect microbial community, while little is known about its effect on viral community. The present study investigated the variation of viral communities, as well as their interactions with microbial hosts under Tl stress. Tl in sediments significantly altered the composition and diversity of the viral communities, but showed no significant links with the prokaryotic communities, which may reveal a potential discrepancy in the sensitivity of the viral and prokaryotic communities to heavy metal stress. Auxiliary metabolic genes (AMGs) involved in denitrification, methane oxidation and organic sulfur transformation were enriched at T1-contaminated sites, while the abundance of AMGs related to methanogenesis and sulfate reduction were higher at pristine sites. Specially, the enrichment of AMGs involved in assimilatory sulfate reduction in Tl-contaminated sites could possibly reduce Tl bioavailability by enhancing the microbially-driven sulfur cycling to generate sulfides that could be complexed with Tl. Moreover, there was a significantly positive correlation between virus-carrying metal resistant genes and the sedimentary Tl concentration, implying that Tl contamination might enhance the metal resistant potential of the viruses. Serving as the functional gene reservoir, the response of viral AMGs to Tl stress could represent a potential pathway for microorganisms to be adapted to the metal-polluted environments. Our study provided novel insights into the impact of Tl spill on viral communities, shedding light on functional characteristics and the links of virus-host interaction with Tl level. © 2024 Elsevier B.V.

关键词： Hazardous materials spills

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Black titanium dioxide nanomaterials for photocatalytic removal of pollutants:A review

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Journal of Materials Science & Technology 2022年第17期112卷 239-262页

作者： Ying Liang Guohe Huang Xiaying Xin Yao Yao Yongping Li Jianan Yin Xiang Li Yuwei Wu Sichen Gao State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentBeijing Normal UniversityBeijing 100875China State Key Joint Laboratory of Environmental Simulation and Pollution Control China-Canada Center for EnergyEnvironment and Ecology ResearchUR-BNUSchool of EnvironmentBeijing Normal UniversityBeijing 100875China Department of Environmental Systems Engineering University of ReginaReginaSKS4S 0A2Canada State Key Laboratory of Marine Pollution(SKLMP) City University of Hong KongKowloonHong Kong SARChina Faculty of Engineering and Applied Science University of ReginaReginaSaskatchewanS4S 0A2Canada

Semiconductor photocatalysis is one of the most widely used environment-friendly technologies for removing various *** a well-developed photocatalyst,titanium dioxide(TiO_(2))still has limits in its wide bandgap and rapid recombination rate of photogenerated charge ***,black TiO_(2)appears as a strong candidate in the improvement of sunlight harvesting,because of its excellent absorption capacity and utilization of solar *** extensive applications in both environmental and energy fields,the use of black TiO_(2)as a photocatalyst in pollutant removal is *** primary objective of the review is to comprehensively evaluate the applications of black TiO_(2)in photocatalytic removal of contaminants,including conventional organic contaminants,emerging contaminants,microbes,and heavy *** basic properties,photocatalytic mechanism,and synthesis of black TiO_(2)have been summarized and ***,the stability and recoverability of black TiO_(2)have also been ***,the perspectives of the application of black TiO_(2)in pollutant removal have been further discussed.

关键词： Photocatalysis Back TiO_(2) Ti^(3+)self-doping Nanomaterials Pollutant removal

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