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Effects of impregnation sequence on the NH_(3)-SCR activity and hydrothermal stability of a Ce-Nb/SnO_(2) catalyst

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Journal of Environmental Sciences 2024年第4期138卷 450-457页

作者： Ying Zhu Wenpo Shan Zhihua Lian Jingjing Liu Yan Zhang hong he Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research StationInstitute of Urban EnvironmentChinese Academy of SciencesNingbo 315800China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

Hydrothermal stability is crucial for the practical application of deNO_(x)catalyst on diesel vehicles,for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).SnO_(2)-based materials possess superior hydrothermal stability,which is attractive for the development of NH_(3)-SCR *** this work,a series of Ce-Nb/SnO_(2)catalysts,with Ce and Nb loading on SnO_(2)support,were prepared by impregnation *** was found that,the NH_(3)-SCR activities and hydrothermal stabilities of the Ce-Nb/SnO_(2)catalysts significantly varied with the impregnation sequences,and the Ce-Nb(f)/SnO_(2) catalyst that firstly impregnated Nb and then impregnated Ce exhibited the best *** characterization results revealed that CeNb(f)/SnO_(2)possessed appropriate acidity and redox ***,the strong synergistic effect between Nb and Sn species stabilized the structure and maintained the dispersion of acid *** study may provide a new understanding for the effect of impregnation sequence on activity and hydrothermal stability and a new environmental-friendly NH_(3)-SCR catalyst with potential applications for NO_(x)removal from diesel and hydrogenfueled engines.

关键词： NO_(x)emission control NH_(3)-SCR Hydrothermal stability Ce-Nb/SnO_(2)catalyst Impregnation sequence

Adsorptive interaction between typical VOCs and various topological zeolites:Mixture effect and mechanism

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Journal of Environmental Sciences 2024年第2期136卷 626-636页

作者： Bo Yu Hua Deng Yuqin Lu Tingting Pan Wenpo Shan hong he 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 State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Adsorption is one of the most feasible and effective methods to alleviate the volatile organic compounds(VOCs)***,the mixture effect and mechanism for competitive adsorption of VOCs on zeolites are barely *** this study,toluene,acetone,and ethyl acetate as prevalent VOCs species were removed by four potential zeolites(13X,USY,Beta,ZSM-5)in both single-and multi-component *** structure-property relationship between adsorbate-adsorbent pairs was revealed by X-ray diffraction,scanning electron microscopy,energy dispersive spectrometer,X-ray fluorescence,N_(2) adsorption and density function theory *** molecular polarity and volatility of VOCs species played key roles in adsorption and the dynamic uptakes were generally listed as follows:ethyl acetate>toluene>*** for the above VOCs mixtures,13X zeolite selectively adsorbed oxygenated VOCs rather than *** contrast,USY exhibited a preference to trap *** acetate could be readily enriched by ZSM-5 and Beta *** possible explanations and implications are discussed based on the subtle change in electron *** results obtained are vital for understanding the mixture effect of VOCs adsorption and may guide the selection of proper adsorbent for real applications.

关键词： Adsorption Zeolites VOCs Mixture effect DFT

Global and regional trends in the incidence and mortality burden of endometrial cancer,1990–2019:Updated results from the Global Burden of Disease Study,2019

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Chinese Medical Journal 2024年第3期137卷 294-302页

作者： Jianyang Feng Rongjin Lin Haoxian Li Jiayan Wang hong he Department of Obstetrics and Gynecology Guangdong Provincial Key Laboratory of Major Obstetric Diseasethe Third Affiliated Hospital of Guangzhou Medical UniversityGuangzhouGuangdong 510000China Department of Fetal Medicine and Prenatal Diagnosis the Third Affiliated Hospital of Guangzhou Medical UniversityGuangzhouGuangdong 510000China

Background:The disease burdens for endometrial cancer(EC)vary across different countries and geographical regions and change every ***,we reported the updated results of the Global Burden of Disease Study 2019 on EC with respect to age-standardized incidence and mortality from 1990 to ***:The annual percentage change(APC)of incidence and mortality was evaluated using joinpoint regression analysis to examine the temporal trends during the same timeframe in terms of the global landscape,different sociodemographic indices(SDI),and geographic *** relationship between Human Development Index(HDI)and incidence and mortality was additionally ***:The age-standardized incidence rates(ASIRs)revealed a significant average global elevation by 0.5%per year(95%confidence interval[CI],0.3–0.7;Phe age-standardized mortality rates(ASMRs),in contrast,fell by an average of 0.8%per year(95%CI,−1.0 to−0.7;Phe ASIR,whereas we detected six consecutively decreasing temporal trends in ASMR during the entire ***,the estimated APCs were significantly positively correlated with HDIs(ρ=0.22;95%CI,0.07–0.35;P=0.003)with regard to incident cases in ***:Incidence rates for EC reflected a significant increase overall(although we observed a decline since 2010),and the death rates declined consecutively from 1990 to *** posit that more precise strategies can be tailored and then implemented based on the distinct age-standardized incidence and mortality burden in different geographical areas.

关键词： Endometrial cancer Global Burden of Disease Incidence Mortality Trends

Carbon allocation in Picea jezoensis:Adaptation strategies of a non-treeline species at its upper elevation limit

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Forest Ecosystems 2024年第3期11卷 347-357页

作者： Renkai Dong Na Li Mai-he Li Yu Cong Haibo Du Decai Gao hong S.he Key Laboratory of Geographical Processes and Ecological Security in Changbai Mountains Ministry of EducationSchool of Geographical SciencesNortheast Normal UniversityChangchun130024China School of Natural Resources University of MissouriColumbiaMO65211USA Swiss Federal Institute for Forest Snow and Landscape Research WSL8903BirmensdorfSwitzerland Northeast Institute of Geography and Agricultural Ecology Chinese Academy of SciencesChangchun130102China School of Life Science Hebei UniversityBaoding071002China

Understanding the physiological adaptations of non-treeline trees to environmental stress is important to understand future shifts in species composition and distribution of current treeline *** aim of the present study was to elucidate the mechanisms of the formation of the upper elevation limit of non-treeline tree species,Picea jezoensis,and the carbon allocation strategies of the species on Changbai *** employed the^(13)C in situ pulse labeling technique to trace the distribution of photosynthetically assimilated carbon in Picea jezoensis at different elevational positions(tree species at its upper elevation limit(TSAUE,1,700 m a.s.l.)under treeline ecotone;tree species at a lower elevation position(TSALE,1,400 m a.s.l.).We analyzed^(13)C and the non-structural carbohydrate(NSC)concentrations in various tissues following *** findings revealed a significant shift in carbon allocation in TSAUE compared to *** was a pronounced increase inδ^(13)C allocation to belowground components(roots,soil,soil respiration)in TSAUE compared to ***,the C flow rate within the plant-soil-atmosphere system was faster,and the C residence time in the plant was shorter in *** trends indicate enhanced C sink activity in belowground tissues in TSAUE,with newly assimilated C being preferentially directed there,suggesting a more conservative C allocation strategy by *** at higher elevations under harsher *** a strategy,prioritizing C storage in roots,likely aids in withstanding winter cold stress at the expense of aboveground growth during the growing season,leading to reduced growth of TSAUE compared to *** results of the present study shed light on the adaptive mechanisms governing the upper elevation limits of non-treeline trees,and enhances our understanding of how non-treeline species might respond to ongoing climate change.

关键词： ^(13)C pulse labeling Carbon distribution Non-structural carbohydrates(NSC) Non-treeline species Sink activity Stressful environments Upper elevation limit

Constructing extrinsic oxygen vacancy on the surface of photocatalyst as CO_(2)and electrons reservoirs to improve photocatalytic CO_(2)reduction activity

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Journal of Environmental Sciences 2024年第6期140卷 37-45页

作者： Zaiyong Jiang Hao Li Zhimin Yuan Zheng Wang Maohong Fan Wenkang Miao hong he State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China School of Chemistry&Chemical Engineering and Environmental Engineering Weifang UniversityWeifangShandong 261061China Departments of Chemical and Petroleum Engineering University of WyomingLaramieWY 82071USA Materials Genome Institute Shanghai UniversityShanghai 200444China

Constructing own oxygen vacancies in the photocatalysts is a very promising method to improve their photocatalytic CO_(2)reduction ***,some catalysts have excellent stabilities,making it difficult for them to construct their own oxygen *** simplify the above difficulty of stable photocatalysts,constructing extrinsic oxygen vacancies on their surface as a novel idea is ***,a stable TiO_(2)nanosheet is chosen as a research object,we uniformly deposited BiOCl quantum dots on their surface via a simple adsorption-deposition *** is found that BiOCl quantum dots are able to simultaneously self-transform into defective BiOCl with many oxygen vacancies when the photocatalyst is performed photocatalytic CO_(2)*** extrinsic oxygen vacancies can act as“CO_(2)and photo-generated electrons reservoirs”to improve CO_(2)capture and accelerate the separation of photogenerated electrons and *** the above reasons,the modified TiO_(2)showed obvious enhancement of photocatalytic CO_(2)reduction compared to pristine TiO_(2)and *** work may open a new avenue to broaden the use of oxygen vacancies in the process of photocatalytic CO_(2)reduction.

关键词： Oxygen vacancy BiOCl Photocatalyst CO_(2)reduction TiO_(2)

Interface sites on vanadia-based catalysts are highly active for NO_(x) removal under realistic conditions

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Journal of Environmental Sciences 2024年第2期136卷 523-536页

作者： Zhihui Lv Guangzhi he Wenshuo Zhang Jingjing Liu Zhihua Lian Yang Yang Zidi Yan Guangyan Xu Wenpo Shan Yunbo Yu hong he State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China Ningbo Research Center for Urban Environment Chinese Academy of SciencesNingbo 315800China

TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic *** these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface *** reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working *** the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O *** wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)*** wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.

关键词： NO_(x)removal Vanadia-based catalysts V-O-Ti entities Interface sites Reaction mechanism

Recent advances in heterogeneous catalysis of solar-driven carbon dioxide conversion

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Journal of Environmental Sciences 2024年第6期140卷 165-182页

作者： Jun Xu Farzaneh Arabpour Roghabadi Ying Luo Vahid Ahmadi Qian Wang Zheng Wang hong he State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China College of Chemistry and Chemical Engineering Henan Polytechnic UniversityJiaozuoHenan 454000China Department of Process Engineering Faculty of Chemical EngineeringTarbiat Modares UniversityTehranIran Optoelectronics and Nanophotonics Research Group Faculty of Electrical and Computer EngineeringTarbiat Modares UniversityTehranIran Graduate School of Engineering Nagoya UniversityFuro-choChikusa-kuNagoya 464-8603Japan

Solar-driven carbon dioxide(CO_(2))conversion including photocatalytic(PC),photoelectrochemical(PEC),photovoltaic plus electrochemical(PV/EC)systems,offers a renewable and scalable way to produce fuels and high-value chemicals for environment and energy *** review summarizes the basic fundament and the recent advances in the field of solar-driven CO_(2)*** the visible-light absorption is an important strategy to improve solar energy conversion *** separation and migration of photogenerated charges carriers to surface sites and the surface catalytic processes also determine the photocatalytic *** engineering including co-catalyst loading,defect engineering,morphology control,surface modification,surface phase junction,and Z-scheme photocatalytic system construction,have become fundamental strategies to obtain high-efficiency *** to photocatalysis,these strategies have been applied to improve the conversion efficiency and Faradaic efficiency of typical PEC *** PV/EC systems,the electrode surface structure and morphology,electrolyte effects,and mass transport conditions affect the activity and selectivity of electrochemical CO_(2)***,the challenges and prospects are addressed for the development of solar-driven CO_(2)conversion system with high energy conversion efficiency,high product selectivity and stability.

关键词： Solar-driven CO_(2)reduction Photocatalytic system Photoelectrochemical system Photovoltaic plus electrochemical system Surface/interface engineering

Promoted NH_(3)-SCR activity and hydrothermal stability of Cu-SSZ-50 catalyst synthesized by one-pot method

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Chinese Chemical Letters 2024年第3期35卷 135-139页

作者： Jinpeng Du Jingyi Wang Yulong Shan Shichao Han Wenpo Shan hong he Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research StationInstitute of Urban EnvironmentChinese Academy of SciencesNingbo 315800China University of Chinese Academy of Sciences Beijing 100049China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Nitrogen oxide(NO_(x))is one of the most critical contaminants in the air,and the control of NO_(x)emission from diesel vehicles is very ***-based small-pore zeolites have already been applied for NO_(x)abatement on diesel *** the small-pore zeolites,Cu-SSZ-50 catalysts with good NH_(3)-SCR catalytic activity were believed to have potential for *** this study,a one-pot synthesis method for Cu-SSZ-50 catalysts was developed for the first time,using the co-templates of Cu-TEPA and 2,6-dimethyl-N-methylpyridinium *** this synthesis method,Cu-SSZ-50 with various Cu contents can be obtained by adjusting the amount of Cu-TEPA without the need for a further after-treatment *** addition of Cu-TEPA affected the framework atoms and Cu species,and a lower Si/Al ratio and more SCR active Cu species were *** synthesized catalyst with a Cu/Al ratio of 0.40 exhibited over 90%NO_(x)conversion between 200℃and 450℃for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).Meanwhile,over 80%NO_(x)conversion could be obtained from 250℃to 450℃after hydrothermal aging at 750℃for 16 *** addition,both L-H and E-R mechanisms were proven to exist for the one-pot-synthesized Cu-SSZ-50 by in situ DRIFTS *** simple synthesis procedure,excellent catalytic activity and hydrothermal stability brighten the prospects for the application of Cu-SSZ-50.

关键词： NH_(3)-SCR Cu-SSZ-50 One-pot synthesis Si/Al ratio Cu species distribution Reaction mechanism

Design of Ca-type todorokite catalysts with highly active for the selective reduction of NO_(x) by NH_(3) at low temperatures

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Journal of Environmental Sciences 2024年第4期138卷 697-708页

作者： Chuang Chang Zidi Yan Chunlei Zhang Yanshuang Zhang Miao Jiang Luna Ruan Min Xiao Yunbo Yu hong he School of Rare Earths University of Science and Technology of ChinaHefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Ca-type todorokite catalysts were designed and prepared by a simple redox method and applied to the selective reduction of NO_(x) by NH_(3)(NH_(3)-SCR)for the first *** with the Na-type manjiroite prepared by the same method,the todorokite catalysts with different Mn/Ca ratios showed greatly improved catalytic activity for NO_(x) *** them,Mn8Ca4 catalyst exhibited the best NH_(3)-SCR performance,achieving 90%NO_(x) conversion within temperature range of 70-275℃ and having a high sulphur *** to the Na-type manjiroite sample,Ca-type todorokite catalysts possessed an increased size of tunnel,resulting in a larger specific surface *** increased the amounts of Ca doping,the Na content in Ca-type todorokite catalysts significantly decreased,providing larger amounts of Bronsted acid sites for NH_(3) adsorption to produce NH_(4)^(+).The NH_(4)^(+)species were highly active for reaction with NO+O_(2),playing a determining role in NH_(3)-SCR process at low ***,larger amounts of surface adsorbed oxygen contained over the Ca-doping samples than that over Na-type manjiroite,promoting the oxidation of NO and fast SCR *** the Ca-type todorokite catalysts,furthermore,nitrates produced during the flow of NO+O_(2),were more active for reaction with NH_(3) than that over Na-type manjiroite,benefiting the occurrence of NH_(3)-SCR *** study provides novel insights into the design of NH_(3)-SCR catalysts with high performance.

关键词： NO_(x) NH_(3)-SCR Mn-based oxides Ca-type todorokite Bronsted acid sites