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Growth of BaTaO_(2)N-BaNa_(0.25)Ta_(0.75)O_(3) Solid Solution Photocatalyst for Visible Light-Driven Z-Scheme Overall Water Splitting

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Energy Material Advances 2022年第1期2022卷 16-23页

作者： Ying Luo Qiaoqi Guo Jun Xu Hanghang Zhou Zheng Wang 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

BaTaO_(2)N with intense visible light absorption has been demonstrated as a promising photocatalyst for Z-scheme overall water splitting,whereas the photocatalytic activity of BaTaO_(2)N is still restricted by strong charge recombination at structural ***,we present the direct growth of BaTaO_(2)N-BaNa_(0.25)Ta_(0.75)O_(3) solid solution from a lattice-matched BaNa_(0.25)Ta_(0.75)O_(3) precursor through volatilization of Na species during a nitridation *** method promotes the direct phase transformation from BaNa_(0.25)Ta_(0.75)O_(3) to BaTaO_(2)N to inhibit the formation of defect *** a result,the as-obtained BaTaO_(2)N-BaNa_(0.25)Ta_(0.75)O_(3) solid solution shows greatly enhanced activity compared to the conventional BaTaO_(2)N,regardless of photocatalytic H2 evolution in the presence of methanol or Z-scheme overall water *** study provides a facile method to construct(oxy)nitride-based solid solution photocatalysts with low defect density for efficient solar hydrogen production from water splitting.

关键词： process catalyst defect

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Cerium-tungsten oxides supported on activated red mud for the selective catalytic reduction of NO_(x)

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Green Energy & environment 2023年第1期8卷 173-182页

作者： Qiuzhun Chen Dong Wang Chuan Gao Bin Wang Shengli Niu Gaiju Zhao Yue Peng Junhua Li Chunmei Lu John Crittenden National Engineering Laboratory for Coal-Burning Pollutants Emission Reduction School of Energy and Power EngineeringShandong UniversityJinan250061China State Key Joint Laboratory of Environment Simulation and Pollution Control National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and EquipmentSchool of EnvironmentTsinghua UniversityBeijing100084China Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering Georgia Institute of Technology828 West Peachtree StreetAtlantaGA30332United States Energy Institute Qilu University of Technology(Shandong Academy of Sciences)Jinan250013ShandongChina

Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of *** inherent low reducibility and acidity limited its low-temperature *** this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based *** activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox *** interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) ***_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid *** Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM ***_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.

关键词： Air pollution control NOx Selective catalytic reduction Cerium Tungsten

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Modeling of wintertime regional formation of secondary organic aerosols around Beijing: sensitivity analysis and anthropogenic contributions

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Carbon Research 2023年第1期2卷 1-19页

作者： Zhang, Yuepeng Huang, Huiying Qin, Weihua Yu, Qing Sun, Yuewei Cheng, Siming Ahmad, Mushtaq Ouyang, Wei Soyol-Erdene, Tseren-Ochir Chen, Jing State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Beijing Normal University Beijing100875 China Center of Atmospheric Environmental Studies Beijing Normal University Beijing100875 China Department of Environmental and Forest Engineering School of Engineering and Applied Sciences National University of Mongolia Ulaanbaatar14201 Mongolia

Modeling of secondary organic aerosol (SOA) has remained a big challenge due to the various precursors and complex processes involved. In this study, the WRF-CAMx model was used to predict the ambient SOA concentrations in urban Beijing as well as the North China Plain (NCP) during a polluted period in winter. To identify the major uncertainties and improve the model performance, a series of model tests were performed to assess the sensitivity of model prediction to the key factors. Then the sources of SOA in Beijing were identified using the optimized model. Both the volatility basis set (VBS) approach and the two-product approach were used for SOA simulation. Although the modeled SOA was underpredicted compared with the SOA estimated through filter-based measurements, the VBS scheme produced higher SOA than the traditional two-product scheme. According to the sensitivity tests with the VBS scheme, the emissions of volatile organic compounds (VOC) and intermediate volatility organic compounds (IVOC) as well as the oxidant levels were the key factors that affected SOA prediction. Based on the optimized simulation scenario, the potential contributions from different anthropogenic sources and source areas were identified, with over 80% of SOA in urban Beijing from regional transport of SOA or its precursors from the surrounding areas during the polluted period. Residential emission in the North China Plain appeared as the dominant source of SOA in urban Beijing from the perspective of regional contribution. Graphical Abstract: [Figure not available: see fulltext.] © 2023, The Author(s).

关键词： Sensitivity analysis

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Effects of persulfate-assisted hydrothermal treatment of municipal sludge on aqueous phase characteristics and phytotoxicity

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Journal of environmental Sciences 2023年第4期126卷 163-173页

作者： Guangchun Shan Weiguang Li Yujie Zhou Shanshan Bao Lin Zhu Wenbing Tan State Key Laboratory of Environmental Criteria and Risk Assessment and State Environmental Protection Key Laboratory of Simulation and Control of Groundwater PollutionChinese Research Academy of Environmental SciencesBeijing 100012China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China Key Laboratory of Water Management and Water Security for Yellow River Basin of Ministry of Water Resources(Under Construction) Yellow River Engineering Consulting Co.LtdZhengzhou 450003China

Hydrothermal technology (HT) has received much attention in recent years as a process to convert wet organic waste into *** aqueous phase (HTAP) produced by this process is still a burden and has become a bottleneck issue for HT process *** this study,we provide the?rst investigation of the HTAP characteristics,phytotoxicity,and their correlation with persulfate (PS)(PS,2.0 mmol/g TS)-assisted municipal sludge *** results showed that PS accelerated the hydrolysis of protein substances and increased the concentration of NH_(4)^(+)by 13.4%to 190.5%and that of PO_(4)^(3-)by 24.2%to 1103.7%in HTAP at hydrothermal temperatures of 120 to 240℃.PS can reduce the phytotoxicity of HTAP by reducing aldehydes,ketones,N heterocyclic compounds,and particle size and by increasing its humi?cation *** maximum values of the root length and biomass of pakchoi(Brassica chinensis L.) seedlings occurred when electrical conductivity was 0.2 mS/cm of *** work provided a new strategy for the selection and design of HTAP management strategies.

关键词： Hydrothermal technology Aqueous phase characteristics Pakchoi Seedlings Phytotoxicity

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A novel photocatalytic mechanism of volatile organic compounds degradation on BaTiO_(3)under visible light:Photo-electrons transfer from photocatalyst to pollutant

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Chinese Chemical Letters 2025年第3期36卷 182-187页

作者： Teng Wang Jiachun Cao Juan Li Didi Li Zhimin Ao Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and Health Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlKey Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of EducationInstitute of Environmental Health and Pollution ControlSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China Advanced Interdisciplinary Institute of Environment and Ecology Guangdong Provincial Key Laboratory of Wastewater Information Analysis and Early WarningBeijing Normal UniversityZhuhai 519087China

Wide bandgap semiconductors are typically activated under ultraviolet(UV)light irradiation for volatile organic compounds(VOCs)***,our previous study discovered that certain VOCs can interact with some wide bandgap semiconductors,formatting an intermediate bandgap between the VOCs and the conduction band of wide bandgap semiconductor,thus inducing visible light activation of the system,and photo-generated electrons are excited by visible light and transferred from the VOCs to the conduction band of *** this work,BaTiO_(3),traditionally is not active under visible light irradiation,however showed degradation rates of 100%and 20%for styrene and toluene under visible light,*** functional theory(DFT)calculations indicate that the adsorption of styrene or toluene on the BaTiO_(3)surface reduces its bandgap from 2.93 eV to 1.36 eV and 2.26 eV,*** intermediate bandgap in this system is primarily formed by the valence band of BaTiO_(3)and the VOCs,and indicating that photo-generated electrons directly transfer from BaTiO_(3)to the VOCs under visible light,inducing degradation reactions of VOCs,i.e.,this work discovered a new transfer pathway of photo-electrons direct from the valence band of BaTiO_(3)to VOCs,while photo-electrons are from VOCs to the conductive band of wide-bandgap semiconductors in our previous work.

关键词： Volatile organic compounds Photocatalytic Degradation Wide-bandgap semiconductors Density functional theory Degradation mechanism

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Delocalization State-Induced C-O Bond Weakness for Enhancing CO2 Electroreduction to Co

SSRN

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SSRN 2024年

作者： Wang, Rong Peng, Yue Chen, Deli Gao, Chuan Wang, Houlin Chen, Zhen Li, Junhua State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China

Manufacturing E-fuels through carbon capture utilization and storage (CCUS), powered by renewable energy conversion, presents a promising pathway towards near-zero emissions for achieving carbon neutrality. However, challenges arise from lower CO selectivity and slower generation rates, leading to suboptimal E-fuels yield and hindering the effective utilization of renewable energy. Drawing inspiration from the hard-soft-based theory, we propose that enhancing the electron delocalization state of catalytic sites can accelerate the CO2 electroreduction to CO. In line with this hypothesis, we have developed a bimetallic catalyst (Ag-Zn) where Ag nanoclusters loaded on ZnO exhibit highly delocalized electrons. Theoretical calculations indicate that Ag-ZnO significantly expedites the hydroxyl detachment of the adsorbed *COOH intermediate, enhancing the efficiency of CO formation. The Ag-ZnO catalyst demonstrates one of the highest CO2-electroreduction-to-CO selectivity (97%) in aqueous electrolyte. Furthermore, our investigation delves into the significance of soft acid sites through in situ X-ray adsorption spectroscopy, in situ Raman spectroscopy and asymmetric low-frequency pulsed strategy. The findings from this study offer theoretical insights guiding the design of catalysts for the efficient electrochemical reduction of CO2 to produce CO. © 2024, The Authors. All rights reserved.

关键词： Electrolytic reduction

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Intensifying electrified flow-through water treatment technologies via local environment modification

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Frontiers of environmental Science & Engineering 2024年第6期18卷 17-25页

作者： Zheng-Yang Huo Xiaoxiong Wang Xia Huang Menachem Elimelech School of Environment and Natural Resources Institute of Ecological CivilizationRenmin University of ChinaBeijing 100872China Institute for Ocean Engineering Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China Center of Double Helix Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Department of Chemical and Environmental Engineering Yale UniversityNew HavenCT 06520-8286USA

Removing high-risk and persistent contaminants from water is challenging,because they typically exist at low concentrations in complex water *** flow-through technologies are viable to overcome the limitations induced by mass transport for efficient contaminant *** the local environment of the flow-through electrodes offers opportunities to further improve the reaction kinetics and selectivity for achieving near-complete removal of these contaminants from ***,we present state-of-the-art local environment modification approaches that can be incorporated into electrified flow-through technologies to intensify water *** first show methods of nanospace incorporation,local geometry adjustment,and microporous structure optimization that can induce spatial confinement,enhanced local electric field,and microperiodic vortex,respectively,for local environment *** then discuss why local environment modification can complement the flow-through electrodes for improving the reaction rate and ***,we outline appropriate scenarios of intensifying electrified flow-through technologies through local environment modification for fit-for-purpose water treatment applications.

关键词： Point-of-use water treatment Electrified membrane Advection-enhanced mass transport Water decontamination and disinfection Emerging contaminants

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Characterization and prediction of tailpipe ammonia emissions from in-use China 5/6 light-duty gasoline vehicles

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Frontiers of environmental Science & Engineering 2024年第1期18卷 71-81页

作者： Lewei Zeng Fengbin Wang Shupei Xiao Xuan Zheng Xintong Li Qiyuan Xie Xiaoyang Yu Cheng Huang Qingyao Hu Yan You Ye Wu College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China State Key Laboratory of Engines Tianjin UniversityTianjin 300072China China Automotive Technology and Research Center Co.Ltd. Tianjin 300300China CATARC Automotive Test Center(Guangzhou)Co.Ltd. Guangzhou 511300China State Environmental Protection Key Laboratory of Cause and Prevention of Urban Air Pollution Complex Shanghai Academy of Environmental SciencesShanghai 200233China National Observation and Research Station of Coastal Ecological Environments in Macao Macao Environmental Research InstituteMacao University of Science and TechnologyMacao SAR 999078China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China

On-road tailpipe ammonia (NH3) emissions contribute to urban secondary organic aerosol formation and have direct or indirect adverse impacts on the environment and human health. To understand the tailpipe NH3 emission characteristics, we performed comprehensive chassis dynamometer measurements of NH3 emission from two China 5 and two China 6 light-duty gasoline vehicles (LDGVs) equipped with three-way catalytic converters (TWCs). The results showed that the distance-based emission factors (EFs) were 12.72 ± 2.68 and 3.18 ± 1.37 mg/km for China 5 and China 6 LDGVs, respectively. Upgrades in emission standards were associated with a reduction in tailpipe NH3 emission. In addition, high NH3 EFs were observed during the engine warm-up period in cold-start cases owing to the intensive emissions of incomplete combustion products and suitable catalytic temperature in the TWCs. Notably, based on the instantaneous NH3 emission rate, distinct NH3–emitting events were detected under high/extra high velocity or rapid acceleration. Furthermore, NH3 emission rates correlated well with engine speed, vehicle specific power, and modified combustion efficiency, which were more easily accessible. These strong correlations were applied to reproduce NH3 emissions from China 5/6 LDGVs. The predicted NH3 EFs under different dynamometer and real-world cycles agreed well with existing measurement and prediction results, revealing that the NH3 EFs of LDGVs in urban routes were within 8.55–11.62 mg/km. The results presented here substantially contribute to improving the NH3 emission inventory for LDGVs and predicting on-road NH3 emissions in China.

关键词： NH3 instantaneous emissions Catalytic temperature Vehicle specific power Combustion efficiency Emission prediction

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Air pollution health burden embodied in China's supply chains

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environmental Science and Ecotechnology 2023年第4期16卷 147-155页

作者： Hongyan Zhao Ruili Wu Yang Liu Jing Cheng Guannan Geng Yixuan Zheng Hezhong Tian Kebin He Qiang Zhang Center for Atmospheric Environmental Studies School of EnvironmentBeijing Normal UniversityBeijing100875China Ministry of Education Key Laboratory for Earth System Modelling Department of Earth System ScienceTsinghua UniversityBeijing100084China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing100084China State Environmental Protection Key Laboratory of Quality Control in Environmental Monitoring China National Environmental Monitoring CentreBeijing100012China Center of Air Quality Simulation and System Analysis Chinese Academy of Environmental PlanningBeijing100012China

Product trade plays an increasing role in relocating production and the associated air pollution impact among sectors and *** a comprehensive depiction of atmospheric pollution redistribution through trade chains is missing,which may hinder targeted clean air cooperation among sectors and ***,we combined five state-of-the-art models from physics,economy,and epidemiology to track the anthropogenic fine particle matters(PM_(2.5))related premature mortality along the supply chains within China in *** results highlight the key sectors that affect PM_(2.5)-related mortality from both production and consumption *** consumption-based effects from food,light industry,equipment,construction,and services sectors,caused 2e22 times higher deaths than those from a production perspective and totally contributed 63%of the national *** a cross-boundary perspective,25.7%of China's PM_(2.5)-related deaths were caused by interprovincial trade,with the largest transfer occurring from the central and northern regions to well-developed east coast *** investment dominated the cross-boundary effect(56%of the total)by involving substantial equipment and construction products,which greatly rely on product exports from regions with specific *** supply chain-based analysis provides a comprehensive quantification and may inform more effective joint-control efforts among associated regions and sectors from a health risk perspective.

关键词： China Air pollution Mortality Trade Supply chain

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Enriching the surface oxygen as efficient anchoring site of highly dispersed Ru for enhanced hydrogenolysis activity

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Nano Research 2023年第10期16卷 12331-12337页

作者： Hongfei Xiao Jianghao Zhang Chuo Du Yanxia Zheng Shuchao Ge Jinhou Fang Shuang Li Changbin Zhang 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 School of Chemical Engineering Northwest UniversityXi’an 710069China Weifang Research Institute of Materials and Technology for Eco-environmental Protection Weifang 261300China

While supported-noble-metal catalysts have been widely investigated in hydrotreating reactions,a crucial issue that the catalytic system is still confronted with is developing an efficient approach to gain the high dispersion of noble metals under reducing *** this work,Ru was supported on two MnOx with different specific surface areas(SSAs),and a much higher dispersion of Ru(83%,in contrast to 42%of the other one)was surprisingly observed over MnO with much lower SSA(around one-third of the other one).A suite of complementary characterizations demonstrates that,compared with the catalyst with high SSA(Ru/MnO-H),the MnO in the one with lower SSA(Ru/MnO-L)contains enriched surface oxygen that creates more abundant sites and bears stronger strength to anchor Ru species,mitigating the aggregation of Ru under reducing *** not only enriched active sites(i.e.,exposed Ru),but also created a more electron-deficient Ru domain and thus enhanced the redox property of the surface,leading to the lower barrier for C–O bond *** the hydrogenolysis of diphenyl ether,Ru/MnO-L exhibited significantly enhanced activity(i.e.,6 folds of Ru/MnO-H)and high *** work provides an approach to regulate the surface chemistry of support for the high dispersion of supported metal.

关键词： anchoring strength oxygen-rich support hydrogenolysis C–O bond cleavage Ru-based catalyst

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