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Smart tailoring of molecular catalysts:Mounting approach to oxygen reduction reaction

Journal of Materials Science & technology 2024年第1期168卷 169-184页

作者： Anuj Kumar Mohd Ubaidullah Guoxin Zhang Jasvinder Kaur Saira Ajmal Mudassir Hasan Krishna Kumar Yadav Hafiz M.Adeel Sharif Ram K.Gupta Ghulam Yasin Nano-technology Research Laboratory Department of ChemistryGLA UniversityMathuraUttar Pradesh 281406India department of Chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia department of Electrical Engineering and Automation Shandong University of Science and TechnologyQingdaoShandong 266590China Institute for Advanced Study Shenzhen UniversityShenzhenGuangdong 518060China department of Chemistry Kansas Polymer Research CenterPittsburg State UniversityPittsburgKS 66762United States Faculty of Science and technology Madhyanchal Professional UniversityRatibadBhopal 462044India environmental and Atmospheric Sciences Research Group Scientific Research CenterAl-Ayen UniversityThi-QarNasiriyah 64001Iraq department of Chemical Engineering King Khalid university Saudi Arabia department of Chemistry School of SciencesIFTM UniversityMoradabadUttar Pradesh 244102India Research Center for Eco-environmental Engineering Dongguan University of TechnologyDongguan 523808China School of Environment and Civil Engineering Dongguan University of TechnologyDongguanGuangdong 523808China

Efficient electrocatalytic rupture of energy-rich molecules(H_(2)and O_(2))is a green approach for gener-ating clean energy for modern *** this context,porphyry-type molecular electrocatalysts act intelligently toward oxygen reduction reaction(ORR),a fundamental process in fuel cells,due to their redox-rich chemistry,which involves core metal ions and macrocyclic *** concerned scientific community has tried many times to correlate the ORR intermediates with their formation kinetics and simplify the associated multi H+/e-stages during the ORR process,constructing several volcano plots be-tween catalytic Tafel data,turnover frequencies,and overpotentials for many *** the fact that many review articles on molecular electrocatalysts for ORR have been published,understanding the strategic implications and molecular catalyst intelligence towards homogenous ORR has been poorly *** review examined the relationships between volcano plots of current *** parameters and the Sabatier principle in order to explain the intelligence of molecular electrocatalysts and approaches for their creation,as well as the difficulties and potential prospects of molecular *** facts distinguish this review from previously published articles and will pique the scien-tific community’s interest in avoiding trial-and-error procedures for catalyst creation while also allowing for more exact evaluations of the molecular catalyst’s performance.

关键词： Electrocatalysis Molecular catalysts Oxygen reduction reaction Sabatier principle

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Recent advances and applications of single atom catalysts based electrochemical sensors

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Nano Research 2024年第4期17卷 2994-3013页

作者： Mingyue Wang Mingfu Ye Jieyue Wang Yong Xu Zhendong Wang Xinyue Tong Xinya Han Kui Zhang Wenhai Wang Konglin Wu Xianwen Wei Institute of Clean energy and Advanced Nanocatalysis(iClean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China School of Materials Science and Engineering Anhui University of TechnologyMaanshan 243002China Anhui International Research Center of energy materials green manufacturing and biotechnology School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Carbon Cycle and Emission Control Research Center Low-Carbon Research InstituteAnhui University of TechnologyMaanshan 243002China

Single atom catalysts(SACs)have attracted considerable attention due to their unique structures and excellent catalytic performance,especially in the area of catalysis science and energy conversion and *** recent years,SACs have emerged as a new type of sensing material for constructing electrochemical sensors(ECSs),presenting excellent sensitivity,selectivity,and ***,we review the recent advances of SACs in electrochemical sensing and discuss the status quo of current SAC-based ***,the fundamentals of SAC-based ECSs are outlined,including the involved central metal atoms and various supports of SACs in this field,the detection mechanisms,and improving strategies of SAC-based ***,the important applications of SAC-based ECSs are listed and classified,covering the detection of reactive oxygen and nitrogen species,environmental pollutants,disease biomarkers,and ***,based on abundant reported cases,the current conundrums of SAC-based ECSs are summarized,and the prediction of their future developing trends is also put forward.

关键词： single atom catalysts(SACs) electrochemical sensors(ECSs) reactive oxygen and nitrogen species environmental pollutants disease biomarkers pharmaceuticals

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Recent progress of two-dimensional metal-base catalysts in urea oxidation reaction

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Rare Metals 2024年第8期43卷 3607-3633页

作者： Qi-Xiang Huang Fang Wang Yong Liu Bi-Ying Zhang Fang-Ya Guo Zhong-Qiu Jia Hao Wang Tian-Xiang Yang Hai-Tao Wu Feng-Zhang Ren Ting-Feng Yi School of Materials Science and Engineering Henan University of Science and TechnologyLuoyang 471000China School of environmental Engineering and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471023China Henan Province International Joint Laboratory of Materials for Solar energy Conversion and Lithium Sodium Based Battery Luoyang 471023China School of Chemistry and Life Sciences Suzhou University of Science and TechnologySuzhou 215009China School of Materials Science and Engineering Northeastern UniversityShenyang110819China

Urea oxidation reaction(UOR)is an auxiliary water electrolysis hydrogen production technology developed in recent years to replace oxygen evolution reaction and reduce energy consumption,which can produce hydrogen more efficiently by low theoretical potential,reduce the average cost of electrochemical hydrogen production,and is a frontier research hotspot for renewable hydrogen ***-dimensional(2D)nanomaterials as electrocatalysts have many favorable potential,such as it can effectively reduce the resistivity of materials and increase the specific surface area with *** paper reviews the application of 2D materials in UOR in alkaline *** a cross-sectional comparison of various material performance data including overpotential,Tafel slope,electrochemical active surface area(ECSA)and it stability test was conducted,which could illustrate the differences between materials composed of different *** addition,the main challenges hindering the progress of research on 2D materials in urea electrocatalysis processes and promising materials in this field in future are summarized and *** is believed that this review will contribute to designing and analyzing highperformance 2D urea electrocatalysts for water splitting.

关键词： Water splitting Urea oxidation reaction Two-dimensional Transition metal compounds Noble/non-noble metals

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A novel insight of degradation ibuprofen in aqueous by catalytic ozonation with supported catalyst:Supports effect on ozone mass transfer

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Journal of environmental Sciences 2024年第11期145卷 216-231页

作者： Zizheng Huangfu Wei Ju Yunhan Jia Ruijun Ren Zhenbei Wang Chen Li Xiaomeng Shang Yujie Li Hongnan Liu YuWang Hao Zheng Fei Qi Amir Ikhlaq Jolanta Kumirska Ewa Maria Siedlecka Beijing Key Laboratory for Source Control technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China Beijing Forestry university Science Co. Ltd.Beijing 100083China Institute of Environment Engineering and Research University of Engineering and TechnologyLahore 54890Pakistan department of environmental Analysis Faculty of ChemistryUniversity of GdanskWita Stwosza 6380-308Poland

Catalytic ozonation is an effective wastewater purification ***,the low ozone mass transfer in packed bubble columns leads to low ozone utilization efficiency(OUE),poor organic degradation performance,and high energy ***,there is an urgent need to develop efficient supported catalysts that can enhancemass transfer and ***,the reaction mechanism of the support on ozone mass transfer remains unclear,which hinders the development of catalytic ozonation *** this study,lava rocks(LR)-supported catalysts,specifically CuMn_(2)O_(4)@LR and MnO_(2)–Co_(3)O_(4)@LR,were proposed for catalytic ozonation of IBP degradation due to their superior catalytic activity,stability,and high *** of CuMn_(2)O_(4)@LR or MnO_(2)–Co_(3)O_(4)@LR increased IBP removal efficiency from 85%to 91%or 88%,and reduced energy consumption from 2.86 to 2.14 kWh/m^(3)or 2.60 kWh/m^(3),*** improvement was attributed to LRsupported catalysts enhancing mass transfer and promoting O3 decomposition to generate•OH and•O_(2)^(−),leading to IBP ***,this study investigated the effects of ozone dose,supporter sizes,and catalyst components on ozone-liquid mass *** results revealed that the size of the supporter influenced stacked porosity and consequently affected ozone mass ***-sized LR(kLa=0.172 min^(−1))exhibited better mass transfer compared to smaller-sized *** on these findings,it was concluded that both CuMn_(2)O_(4)@LR and MnO_(2)–Co_(3)O_(4)@LR are potential catalysts for catalytic ozonation in residual IBP degradation of pharmaceutical wastewater,and LR showed good credibility as a catalyst *** the effects of supporters and active components on ozone mass transfer provides a fundamental principle for designing supported catalysts in catalytic ozonation applications.

关键词： Catalytic ozonation Lava rocks Overall volumetric mass transfer coefficient Supported catalyst

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Singlet oxygen-dominated peroxymonosulfate activation by layered crednerite for organic pollutants degradation in high salinity wastewater

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Journal of environmental Sciences 2024年第1期135卷 86-96页

作者： Chengji Sui Zixuan Nie Huan Liu Grzegorz Boczkaj Weizhen Liu Lingshuai Kong Jinhua Zhan Key Laboratory for Colloid&Interface Chemistry of Education Ministry Department of ChemistryShandong UniversityJinan 250100China School of Environment and energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and RecyclingSouth China University of TechnologyGuangzhou 510006China Gdansk university of technology Faculty of Civil and Environmental EngineeringDepartment of Sanitary EngineeringG.Narutowicza St.11/1280-233 GdanskPoland EkoTech Center Gdansk University of TechnologyG.Narutowicza St.11/1280-233 GdanskPoland

Advanced oxidation processes have been widely studied for organic pollutants treatment in water,but the degradation performance of radical-dominated pathway was severely inhibited by the side reactions between the anions and radicals,especially in high salinity ***,a singlet oxygen(^(1)O_(2))-dominated non-radical process was developed for organic pollutants degradation in high salinity wastewater,with layered crednerite(CuMnO_(2))as catalysts and peroxymonosulfate(PMS)as *** on the experiments and density functional theory calculations,^(1)O_(2)was the dominating reactive species and the constructed Cu-O-Mn with electron-deficient Mn captured electron from PMS promoting the generation of^(1)O_(2).The rapid degradation of bisphenol A(BPA)was achieved by CuMnO_(2)/PMS system,which was 5-fold and 21-fold higher than that in Mn_(2)O_(3)/PMS system and Cu_(2)O/PMS *** CuMnO_(2)/PMS system shown prominent BPA removal performance under high salinity conditions,prominent PMS utilization efficiency,outstanding total organic carbon removal rate,wide range of applicable pH and good *** work unveiled that the^(1)O_(2)-dominated non-radical process of CuMnO_(2)/PMS system overcame the inhibitory effect of anions in high salinity conditions,which provided a promising technique to remove organic pollutants from high saline wastewater.

关键词： Singlet oxygen Non-radical process High salinity Mixed metal oxides Wastewater treatment

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Potential industrial applications of photo/electrocatalysis: Recent progress and future challenges

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Green energy & Environment 2024年第5期9卷 859-876页

作者： Jinhao Li Jing Ren Shaoquan Li Guangchao Li Molly Meng-Jung Li Rengui Li Young Soo Kang Xiaoxin Zou Yong Luo Bin Liu Yufei Zhao State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou324000China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China department of Applied Physics The Hong Kong Polytechnic UniversityHong Kong999077China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian National Laboratory for Clean EnergyZhongshan Road 457Dalian116023China environmental and Climate technology Track of Korea Institute of energy Korea Institute of Energy TechnologyNaju-siJeollanam do58217Republic of Korea State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun130012China

Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental *** this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis technology for the advantage in the sustainable production of high-value-added products,and the high efﬁciency in pollutants *** there is plenty of outstanding research has been put forward continuously,most of them focuses on catalysis performance and reaction mechanisms in laboratory *** industrial application of photo/electrocatalytic processes is still a challenge that needs to be overcome by social *** this regard,this review comprehensively summarized several explorations in theﬁeld of photo/electrocatalytic reduction towards potential industrial applications in recent *** attention is paid to the successful attempts and the current status of photo/electrocatalytic water splitting,carbon dioxide conversion,resource utilization from waste,etc.,by using advanced *** key problems and challenges of photo/electrocatalysis in future industrial practice are also discussed,and the possible development directions are also pointed out from the industry view.

关键词： Photocatalysis Electrocatalysis Industrial applications H2 economy

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A mixed-valence polyoxometalate-based 3D inorganic framework cathode material for high-efficiency rechargeable AZIBs

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Rare Metals 2024年第8期43卷 3677-3691页

作者： Qing Han Hao-Ran Xiao Tao Zhou Bing-Chuan Li Liu Yang Ling-Ling Xie Xue-Jing Qiu Xian-Yong Wu Li-Min Zhu Xiao-Yu Cao School of Chemistry and Chemical Engineering Henan University of TechnologyZhengzhou 450001China Key Laboratory of High Specific energy Materials for Electrochemical Power Sources of Zhengzhou City Zhengzhou 450001China College of Materials Engineering Henan University of EngineeringZhengzhou450007China School of environmental Engineering Henan University of TechnologyZhengzhou 450001China department of Chemistry University of Puerto Rico-Rio Piedras CampusSan JuanPR 00925USA

The global trend towards new energy storage systems has stimulated the development of electrochemical energy storage *** these technologies,rechargeable aqueous zinc-ion batteries(AZIBs)have attracted considerable interest as a potential alternative to lithium-ion batteries(LIBs)due to their affordable cost,environmental compatibility and high safety *** this study,a high-quality electrode for AZIBs has been successfully developed using a dehydrated mixed-valence polyoxometalate-based three-dimensional(3D)inorganic framework material known as[H_6Mn_(3)V^Ⅳ_(15)V-^Ⅴ_(4O)_(46)(H_2O)_(12)](3D-MnVO).This innovative 3D-MnVO material is built from the alternate connections of{V_(19)O_(46)}"sphere-shaped"clusters andμ_(2)-{Mn(H_(2)O)_(4)}bridges,where each{V_(19)O_(46)}cluster is surrounded by three pairs of vertically distributed{Mn(H_(2)O)_(4)}units,thus resulting in the 3D interpenetrating grid-like network from the infinite[-{V_(19)O_(46)}-μ_(2)-Mn(H_(2)O)_(4)-{V_(19)O_(46)}]_∞chains in three mutually perpendicular *** 3D framework structure of 3D-MnVO possesses abundant oxygen vacancies,spacious and multi-level interconnected channels for ion transport,which facilitates the efficient intercalation/deintercalation of hydrated Zn^(2+)into the pores of the primary structure via the intercalation capacitance *** a result,the 3D-MnVO electrode exhibits excellent diffusion rates and minimal interfacial *** a current density of 0.1 A·g^(-1),the 3D-MnVO cathode delivers a commendable discharge capacity of170.5 mAh·g^(-1)with 81.6%capacity retention after100 charge/discharge ***,even at a high current density of 1.0 A·g^(-1),the 3D-MnVO electrode delivers a remarkable reversible capacity of198.9 mAh·g^(-1).Our research results provide valuable insights into the development of advanced polyoxometalate-based 3D inorganic framework electrode materials for high-performance rechargeable AZIBs.

关键词： Cathode Polyoxometalate 3D inorganic framework Zinc-ion batteries energy storage mechanism

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Experimental and theoretical insight into carbamazepine degradation by chlorine-based advanced oxidation processes:Efficiency,energy consumption,mechanism and DBPs formation

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Journal of environmental Sciences 2024年第5期139卷 72-83页

作者： Chunwei Liu Zuo Tong How Yue Ju Li Feng Xuefeng Ren Mohamed Gamal El-Din Key Laboratory ofCoal Processing and Efficient Utilization of Ministry of Education School of Chemical Engineering and TechnologyChina University of Mining and TechnologyJiangsu 221116China department of Civil and environmental Engineering University of AlbertaEdmonton T6G 1H9AlbertaCanada School of Environment and Spatial Informatics China University of Mining and TechnologyJiangsu 221116China Key Laboratory of Agro-Forestry environmental Processes and Ecological Regulation ofHainan Province School of Ecology and EnvironmentHainan UniversityHainan 570228China

Chlorine has been widely used in different advanced oxidation processes(AOPs)for micropollutants *** this study,different chlorine-based AOPs,namely medium pressure(MP)UV/chlorine,low pressure(LP)UV/chlorine,and in-situ chlorination,were compared for carbamazepine(CBZ)removal efficiency,energy consumption,and disinfection by-products(DBPs)*** three processes could achieve nearly 100%CBZ removal,while the reaction time needed by in-situ chlorination was double the time required by UV/chlorine *** energy consumed per magnitude of CBZ removed(EE/O)of MP UV/chlorine was 13 times higher than that of LP UV/chlorine,and relative to that of in-situ chlorination ***,MP and LP UV/chlorine processes generated one to two orders of magnitude more hydroxyl radicals(^(·)OH)and reactive chlorine species(RCS)than in-situ ***,RCS were the dominant reactive species,contributing to 78.3%,75.6%,and 71.6% of CBZ removal in MP,LP UV/chlorine,and in-situ chlorination,*** to the Gibbs free energy barriers between CBZ and RCS/^(·)OH calculated based on density functional theory(DFT),RCS had more reaction routes with CBZ and showed lower energy barrier in the main CBZ degradation pathways like epoxidation and formation of *** applied to secondary wastewater effluent,UV/chlorine and in-situ chlorination produced overall DBPs ranging from 104.77 to 135.41μg/***,the production of chlorate during UV/chlorine processes was 15 times higher than that during in-situ chlorination.

关键词： UV/chlorine In-situ chlorination energy efficiency Role of reactive species DFT calculation Disinfection by-products

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

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Frontiers in energy 2024年第2期18卷 128-140页

作者： Junwen CAO Yikun HU Yun ZHENG Wenqiang ZHANG Bo YU Institute of Nuclear and New energy technology(INET) Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijing 100084China department of Chemical Engineering University of WaterlooWaterlooOntario N2L 3G1Canada Institute of New energy Materials and Engineering School of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China

The Haber-Bosch process is the most widely used synthetic ammonia technology at *** its invention,it has provided an important guarantee for global food ***,the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental *** the serious pressure of energy and environment,a green,clean,and sustainable ammonia synthesis route is urgently *** synthesis of ammonia is a green and mild new method for preparing ammonia,which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar,wind,or water energy,without greenhouse gas and toxic gas ***,the basic mechanism of the nitrogen reduction reaction(NRR)to ammonia and nitrate reduction reaction(NO_(3)^(-))to ammonia were *** representative approaches and major technologies,such as lithium mediated electrolysis and solid oxide electrolysis cell(SOEC)electrolysis for NRR,high activity catalyst and advanced electrochemical device fabrication for(NO_(3)^(-))RR and electrochemical ammonia synthesis were *** on the above discussion and analysis,the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis nitrogen nitrate nitrogen reduction reaction(NRR)to ammonia nitrate reduction reaction(NO_(3)^(-))RR

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Ambient formaldehyde concentrations in summer in 30 Chinese cities and impacts on air cleaning of built environment

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energy and Built Environment 2024年第4期5卷 493-499页

作者： Shuolin Qiu Zirui He Guangdong Liu Zhen Ding Zhongming Bu Jianping Cao Wenjing Ji Wei Liu Chunxiao Su Xinke Wang Fan Liu Ting Li Hua Qian Cong Liu School of energy and Environment Southeast UniversityNanjingJiangsu210096China China Green Development Investment Group Co.LTD Beijing100000China department of environmental Health Jiangsu Provincial Center for Disease Control and PreventionNanjingJiangsu210009China department of energy and environmental System Engineering Zhejiang University of Science and TechnologyHangzhouZhejiang310023China School of environmental Science and Engineering Sun Yat-sen UniversityGuangzhouGuangdong510006China School of Civil and Resource Engineering University of Science and Technology BeijingBeijing100083China Institute for Health and Environment Chongqing University of Science and TechnologyChongqing401331China School of Environment and Architecture University of Shanghai for Science and TechnologyShanghai200093China School of Human Settlements and Civil Engineering Xi’an Jiaotong UniversityXi’an710049ShaanxiChina Tsinghua university Beijing100084China

Formaldehyde is an important carcinogen commonly found *** indoor sources have been intensively *** study on outdoor formaldehyde concentration,which is potentially an important source to indoors,remains *** study attempts to characterize temporal and spatial distribution of the atmospheric formalde-hyde concentration in Chinese *** variation of ambient formaldehyde was examined in 6 cities and peak hours were identified between 12:00 pm and 3:00 ***,outdoor formaldehyde concentrations were measured in the peak hours in 30 cities during the summer months of Jul.-Aug.,*** formaldehyde concentrations in the peak hours fell into a range of 0.005-0.087 mg/m^(3)(median value is 0.027 mg/m^(3)),87.7%of which have exceeded the chronic reference exposure criteria of 0.009 mg/m^(3) set by Office of environmental Health Hazard *** risk analysis suggests that exposure to ambient formaldehyde could cause a median carcinogenic risk of 1.9×10^(−5)(3.17×10^(−6)-6.13×10^(−5)),higher than threshold limit of 10−*** correlation analysis of the 30 cities shows that ambient summertime atmospheric formaldehyde concentrations of the city are positively correlated with its Gross Domestic Product(r=0.48).We also found that the outdoor formaldehyde concentrations in urban areas(median:0.017 mg/m^(3))is slightly higher than those in suburban areas(median:0.013 mg/m^(3)).Results here prove that outdoor formaldehyde is ubiquitous in Chinese cities and reduces effectiveness of ventilation in dilution indoor *** it would underestimate air cleaner capacity needed by a factor of about *** should be accounted for in health analysis and air quality engineering control design of built environment in the future.

关键词： Atmospheric formaldehyde Temporal distribution Health risk Ventilation efficiency

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