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Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane

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Angewandte Chemie 2023年第39期135卷

作者： Shimao Deng Ranhao Wang Xuezhen Feng Dr. Renji Zheng Shaokuan Gong Prof. Xihan Chen Yangzi Shangguan Lili Deng Huan Tang Hao Dai Prof. Lele Duan Prof. Chengyuan Liu Prof. Yang Pan Prof. Hong Chen State Environmental Protection Key Laboratory of Integrated Surface Water Groundwater Pollution Control Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control Key Laboratory of Municipal Solid Waste Recycling Technology and Management of Shenzhen City Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (SKLISEM) School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen 518055 China SUSTech Energy Institute for Carbon Neutrality Department of Mechanical and Energy Engineering Southern University of Science and Technology Shenzhen 518055 China Department of Chemistry Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology Shenzhen 518055 China National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 China

Highly selective photoreduction of CO 2 to valuable hydrocarbons is of great importance to achieving a carbon-neutral society. Precisely manipulating the formation of the Metal 1 ⋅⋅⋅C=O⋅⋅⋅Metal 2 (M 1 ⋅⋅⋅C=O⋅⋅⋅M 2 ) intermediate on the photocatalyst interface is the most critical step for regulating selectivity, while still a significant challenge. Herein, inspired by the polar electronic structure feature of CO 2 molecule, we propose a strategy whereby the Lewis acid-base dual sites confined in a bimetallic catalyst surface are conducive to forming a M 1 ⋅⋅⋅C=O⋅⋅⋅M 2 intermediate precisely, which can promote selectivity to hydrocarbon formation. Employing the Ag 2 Cu 2 O 3 nanowires with abundant Cu⋅⋅⋅Ag Lewis acid-base dual sites on the preferred exposed {110} surface as a model catalyst, 100 % selectivity toward photoreduction of CO 2 into CH 4 has been achieved. Subsequent surface-quenching experiments and density functional theory (DFT) calculations verify that the Cu⋅⋅⋅Ag Lewis acid-base dual sites do play a vital role in regulating the M 1 ⋅⋅⋅C=O⋅⋅⋅M 2 intermediate formation that is considered to be prone to convert CO 2 into hydrocarbons. This study reports a highly selective CO 2 photocatalyst, which was designed on the basis of a newly proposed theory for precise regulation of reaction intermediates. Our findings will stimulate further research on dual-site catalyst design for CO 2 reduction to hydrocarbons.

关键词： Ag⋅⋅⋅C=O⋅⋅⋅Cu Intermediate Lewis Acid-Base Dual Sites Methane Selective Reduction

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Publisher Correction: Ozone pollution mitigation strategy informed by long-term trends of atmospheric oxidation capacity

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Nature Geoscience 2024年 172页

作者： Wenjie Wang Xin Li Ying Liu Sihua Lu Yusheng Wu Shiyi Chen Keding Lu Min Hu Limin Zeng Min Shao Yuanhang Zhang Hang Su Yafang Cheng Ruijing Ni Ulrich Pöschl Zhaofeng Tan Franz Rohrer Andreas Wahner David D. Parrish Cheng Huang Xudong Tian K. M. Leung Liangfu Chen Meng Fan Qiang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing China State Key Laboratory of Atmospheric Environment and Extreme Meteorology Institute of Atmospheric Physics Chinese Academy of Sciences Beijing China Max Planck Institute for Chemistry Mainz Germany International Joint Laboratory for Regional Pollution Control Ministry of Education Beijing China Collaborative Innovation Centre of Atmospheric Environment and Equipment Technology Nanjing University of Information Science & Technology Nanjing China Institute of Carbon Neutrality Peking University Beijing China Institute for Environmental and Climate Research Jinan University Guangzhou China State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex Shanghai Academy of Environmental Sciences Shanghai China Institut für Energie-und Klimaforschung: Troposphäre (IEK-8) Forschungszentrum Jülich Jülich Germany Key Laboratory of Ecological and Environmental Monitoring Forewarning and Quality Control of Zhejiang Zhejiang Ecological and Environmental Monitoring Center Hangzhou China Environmental Protection Department The Government of the Hong Kong Special Administrative Region Hong Kong China State Key Laboratory of Remote Sensing Science The Aerospace Information Research Institute Chinese Academy of Sciences Beijing China Department of Earth System Science Tsinghua University Beijing China

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Impact of Biomass Burning on Pm2.5 Concentrations Over Northeast Asia: Insights from Quantitative Estimates and Spatial Distributions of Biomass Burning Aerosols

SSRN

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SSRN 2023年

作者： Nirmalkar, Jayant Song, Mijung Lee, Ji Yi Lee, Kwangyul Ahn, Junyoung Qiu, Yanting Wu, Zhijun Natsagdorj, Amgalan Jang, Kyoung-Soon Kim, Changhyuk Department of Earth and Environmental Sciences Jeonbuk National University Jeonju54896 Korea Republic of Department of Environmental Science and Engineering Ewha Womans University Seoul03760 Korea Republic of Division of Climate and Air Quality Research National Institute of Environmental Research Incheon22689 Korea Republic of State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing100871 China Department of Chemistry School of Arts and Sciences National University of Mongolia Ulaanbaatar14201 Mongolia Bio-Chemical Analysis Team Korea Basic Science Institute Cheongju28119 Korea Republic of School of Civil and Environmental Engineering Pusan National University Busan46241 Korea Republic of Department of Environment and Energy Jeonbuk National University Jeonju54896 Korea Republic of

To the best of our knowledge, for the first time an extensive study was undertaken to comprehensively understand the simultaneous quantitative estimates of biomass burning (BB) aerosol in fine particulate matter (PM2.5) in four different sites including both metropolitan and rural areas of Northeast Asia during spring. PM2.5 were simultaneously collected in Seoul and Seosan (SE and SS, Korea, respectively), Beijing (BJ, China) and Ulaanbaatar (UB, Mongolia), spanning from March to April 2022. These collected samples were analyzed to identify and quantify BB markers, including levoglucosan, mannosan, K+ and organic carbon (OC). This analysis aimed to provide valuable insights into the impact and contribution of BB to PM2.5 and OC. Using the ratios of levoglucosan/K+ and levoglucosan/mannosan, we showed that the contribution of OC-BB to the total OC varied significantly among the sites, with SE showing a contribution of 27% ± 17%, SS 60% ± 24%, BJ 4% ± 3%, and UB 50% ± 17%. Concentrations of levoglucosan and OC-BB were highest at UB and SS sites, indicating a greater impact of BB aerosol compared to SS and BJ. Cluster and Potential Source Contribution Function analyses showed that in the SE site, aerosols were influenced by BB aerosols originating from both the northwest and south directions. Conversely, in the SS area, the study detected the presence of aged, regional, and long-range transported aerosols from the northwest and south directions. In addition, our study focused on deriving an optimized OC/levoglucosan ratio, which is crucial for the accurate estimation of OC-BB concentrations. Moreover, the approach utilized in this study can be applied in other regions to estimate region-specific OC ∕ levoglucosan ratios for OC-BB and aid in the establishment of targeted BB control measures, thereby improving air quality and environmental protection. © 2023, The Authors. All rights reserved.

关键词： Organic carbon

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The China groundwater crisis: A mechanistic analysis with implications for global sustainability

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Sustainable Horizons 2022年 4卷

作者： Lancia, Michele Yao, Yingying Andrews, Charles B. Wang, Xiaoli Kuang, Xingxing Ni, Jinren Gorelick, Steven M. Scanlon, Bridget R. Wang, Yanxin Zheng, Chunmiao State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen China EIT Institute for Advanced Study Ningbo China Department of Earth and Environmental Sciences School of Human Settlements and Civil Engineering Xi'an Jiaotong University Xi'an China S.S. Papadopulos & Associates Inc. RockvilleMD United States Department of Civil Engineering The University of Hong Kong Hong Kong Hong Kong College of Environmental Sciences and Engineering Peking University Beijing China Department of Earth System Science Stanford University StanfordCA United States Bureau of Economic Geology Jackson School of Geosciences University of Texas at Austin AustinTX United States China University of Geosciences Wuhan China

Over the past several decades, China has rapidly depleted groundwater storage, and has lagged in managing and protecting this resource. As a result, dried up rivers, land subsidence, saltwater intrusion, and wetland losses are extensive. To assist with managing this vital groundwater resource, we constructed the first national-scale numerical groundwater flow model of China to provide a comprehensive overview and understanding of the subsurface flow dynamics. The groundwater model is three-dimensional with a 10 km by 10 km horizontal resolution and five discretized vertical layers (up to 1700 m below the land surface). The calibrated model matched calculated to observed water levels and sufficiently reproduced water budgets. The model was used to reconstruct groundwater depletion by retracing the different stages of Chinese economic development. From 1945 to 2020, the northern provinces are characterized by an average groundwater depletion of ∼16.7 km3/yr (equivalent to 30% of the Yellow River's annual flow) while southern China has experienced no substantial groundwater depletion. groundwater depletion is consistent with a large observed reduction in groundwater discharge as baseflow to the Yellow River (-23%) relative to negligible variation in baseflow in the Yangtze River. Our study provides a holistic tool to support development of nationwide water management strategies and temper the effects of a future water crisis that China's growing economy could propagate at the global scale. © 2022

关键词： groundwater resources

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Sources of atmospheric glyoxal and methylglyoxal in Beijing and its impact on wintertime secondary organic aerosol formation

Sources of atmospheric glyoxal and methylglyoxal in Beijing ...

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第二十四届大气污染防治技术研讨会

作者： Xionghui Qiu Shuxiao Wang Qi Ying Lei Duan Jia Xing Jingyuan Cao Di Wu Xiaoxiao Li Chengzhi Xing Xiao Yan Cheng Liu Jiming Hao MOE Key Laboratory of Resources and Environmental System Optimization College of Environmental Science and Engineering North China Electric Power University State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Zachry Department of Civil Engineering Texas A&M University College Station School of Earth and Space Sciences University of Science and Technology of China National Engineering Research Center of Urban Environmental Pollution Control Beijing Municipal Research Institute of Environmental Protection Department of Precision Machinery and Precision Instrumentation University of Science and Technology of China

Atmospheric glyoxal(GLY) and methylglyoxal(MGLY) are key precursors of secondary organic aerosol(SOA). However, anthropogenic emissions of GLY and MGLY and their contribution to surface GLY and MGLY concentrations, as well as the secondary organic aerosol(SOA) formation, are not well quantified. By developing an emission inventory of anthropogenic GLY and MGLY and improving Community Multiscale Air Quality Model(CMAQ) with SOA formation from irreversible surface uptake of GLY and MGLY, as well as a precursor-origin resolved technique, we quantified the source contributions of GLY and MGLY and their impact on wintertime SOA formation in Beijing, China. The total emissions of GLY and MGLY in Beijing in 2017 are 1.1×10～4 kmol and 7.0×10～3 kmol, respectively. Anthropogenic primary emissions are found to be the dominant contributor to GLY and MGLY concentrations(～74% for GLY and ～63% for MGLY). Anthropogenic primary emissions of GLY and MGLY contributes to 30% of GLY/MGLY SOA daily average concentration and accounts for up to 45% of nighttime GLY/MGLY SOA. The study suggests that the anthropogenic GLY and MGLY emissions, mainly from gasoline vehicles and cooking, are important for SOA formation and shall be strictly controlled in Chinese megacities.

关键词： SOA Sources of atmospheric glyoxal and methylglyoxal in Beijing and its impact on wintertime secondary organic aerosol formation

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Coextraction of vanadium and manganese from highmanganese containing vanadium wastewater by a solvent extraction-precipitation process

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Frontiers of Chemical Science and Engineering 2020年第5期14卷 902-912页

作者： Zishuai Liu Yimin Zhang Zilin Dai Jing Huang Cong Liu School of Resource and Environmental Engineering Wuhan University of Science and TechnologyWuhan 430081China Guangdong Research Institute of Rare-Metal Guangzhou 510650China State Environmental Protection Key Laboratory of Mineral Metallurgical Resources Utilization and Pollution Control Wuhan University of Science and TechnologyWuhan 430081China Hubei Collaborative Innovation Center for High Efficient Utilization of Vanadium Resources Wuhan University of Science and TechnologyWuhan 430081China Hubei Provincial Engincering Technology Research Center of High Eficient Cleaning Uilization for Shale Vanadium Resources Wuhan University of Science and TechnologyWuhan 430081China

High-manganese containing vanadium waste-water(HMVW)is commonly produced during the vanadium extraction process from vanadium *** cannot be reused and discharged directly,and is harmful to the environment and affect product quality due to heavy metals in the *** wastewater is usually treated by lime neutralization,but valuable metals(especially V and Mn)cannot be *** this study,an efficient and environmentally friendly method was developed to recover valuable metals by using a solvent extraction-precipitation *** the solvent extraction process,98.15%of vanadium was recovered,and the V2Os product,with a purity of 98.60%,was obtained under optimal *** the precipitation process,91.05%of manganese was recovered as MnCO3 which meets the III grade standard of HG/T *** simulation analysis indicated that MnCO3 was selectively precipitated at pH 6.5 while Mg and Ca could hardly be *** results of X-ray diffraction and scanning electron microscopy demonstrated that the obtained V2Os and MnCO3 displayed a good degree of *** treated wastewater can be returned for leaching,and resources(V and Mn)in the wastewater were utilized efficiently in an environmentally friendly ***,this study provides a novel method for the coextraction of V and Mn from HMVW.

关键词： high-manganese containing vanadium waste-water solvent extraction carbonate precipitation vanadium titano-magnetite valuable metal recovery

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Corrigendum to “Dynamic scouring of multifunctional granular material enhances filtration performance in membrane bioreactor: Mechanism and modeling” [J. Membr. Sci. 663 (2022) 120979]

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Journal of Membrane Science 2024年 698卷

作者： Wenxiang Zhang Wenzhong Liang Zhien Zhang Biological and Environmental Science and Engineering Division Water Desalination and Reuse Research Center King Abdullah University of Science and Technology Thuwal Saudi Arabia State Environmental Protection Key Laboratory of Water Environmental Simulation and Pollution Control South China Institute of Environmental Sciences Ministry of Ecology and Environment of the People's Republic of China Guangzhou 510530 PR China Department of Chemical and Biomedical Engineering West Virginia University 40110 Evansdale Drive Morgantown WV 26506 USA

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Deep-learning based discovery of partial differential equations in integral form from sparse and noisy data

arXiv

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arXiv 2020年

作者： Xu, Hao Zhang, Dongxiao Wang, Nanzhe BIC-ESAT ERE and SKLTCS College of Engineering Peking University Beijing100871 China Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen518055 China State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen518055 China Intelligent Energy Lab Peng Cheng Laboratory Shenzhen518000 China

Data-driven discovery of partial differential equations (PDEs) has attracted increasing attention in recent years. Although significant progress has been made, certain unresolved issues remain. For example, for PDEs with high-order derivatives, the performance of existing methods is unsatisfactory, especially when the data are sparse and noisy. It is also difficult to discover heterogeneous parametric PDEs where heterogeneous parameters are embedded in the partial differential operators. In this work, a new framework combining deep-learning and integral form is proposed to handle the above-mentioned problems simultaneously, and improve the accuracy and stability of PDE discovery. In the framework, a deep neural network is firstly trained with observation data to generate meta-data and calculate derivatives. Then, a unified integral form is defined, and the genetic algorithm is employed to discover the best structure. Finally, the value of parameters is calculated, and whether the parameters are constants or variables is identified. Numerical experiments proved that our proposed algorithm is more robust to noise and more accurate compared with existing methods due to the utilization of integral form. Our proposed algorithm is also able to discover PDEs with high-order derivatives or heterogeneous parameters accurately with sparse and noisy data. © 2020, CC-BY-NC-ND.

关键词： Partial differential equations

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Mercury flows in large-scale gold production and implications for Hg pollution control

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Journal of environmental Sciences 2018年第6期30卷 91-99页

作者： Qingru Wu Shuxiao Wang Mei Yang Haitao Su Guoliang Li Yi Tang Jiming Hao State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084 China College of Electromechanical Engineering Qingdao University of Science and Technology Qingdao 266061 China

Large-scale gold production（LSGP） is one of the five convention-related atmospheric mercury（Hg） emission sources in the Minamata Convention on Mercury. However, field experiments on Hg flows of the whole process of LSGP are limited. To identify the atmospheric Hg emission points and understand Hg emission characteristics of LSGP, Hg flows in two gold smelters were studied. Overall atmospheric Hg emissions accounted for 10%–17% of total Hg outputs and the Hg emission factors for all processes were 7.6–9.6 kg/ton. There were three dominant atmospheric Hg emission points in the studied gold smelters, including the exhaust gas of the roasting process, exhaust gas from the environmental fog collection stack and exhaust gas from the converter of the refining process. Atmospheric Hg emissions from the roasting process only accounted for 16%–29% of total emissions and the rest were emitted from the refining process. The overall Hg speciation profile（gaseous elemental Hg/gaseous oxidized Hg/particulate-bound Hg） for LSGP was 34.1/57.1/8.8. The dominant Hg output byproducts included waste acid, sulfuric acid and cyanide leaching residue. Total Hg outputs from these three byproducts were 80% in smelter A and 84% in smelter B. Our study indicated that previous atmospheric Hg emissions from large-scale gold production might have been *** emission control in LSGP is not especially urgent in China compared to other significant emission sources（e.g., cement plants）. Instead, LSGP is a potential Hg release source due to the high Hg output proportions to acid and sludge.

关键词： Large-scale gold production Mercury Flow analysis Emission characteristics

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Effect of ozone injection on the long-term performance and microbial community structure of a VOCs biofilter

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Journal of environmental Sciences 2018年第7期30卷 133-140页

作者： Prakit Saingam Zenab Baig Yang Xu Jinying Xi Environmental Simulation and Pollution Control State Key Joint Laboratory School of Environment Tsinghua University Key Laboratory of Microorganism Application and Risk Control of Shenzhen Graduate School at Shenzhen Tsinghua University

For biofilters treating waste gases containing volatile organic compounds（VOCs）, biomass accumulation is a common problem which will induce bed clogging and significant decrease in VOCs removal efficiency during long-term operation. In this study, ozone injection was developed as a biomass control strategy, and its effects on the biofilter performance and the microbial community structure were investigated in long-term operation. Two biofilters,identified as BF1 and BF2, were operated continuously for 160 days treating gaseous toluene under the same conditions, except that 200 mg/m^3 ozone was continuously injected into BF1 during days 45–160. During the operation period, ozone injection did not change the toluene removal efficiency, while the pressure drop of BF1 with ozone injection was significantly lowered compared with BF2. The wet biomass accumulation rate of BF1 was 11 g/m^3/hr, which was only46% of that in BF2. According to the carbon balance result, ozone injection also increased the toluene mineralization rate from 83% to 91%, which could be an important reason for the low biomass accumulation. The PMA-q PCR result indicated that ozone injection increased the microbial viability of the biofilm. The high-throughput sequencing result also revealed that the dominant phyla and genera were not changed significantly by ozone injection, but some ozonetolerant genera such as Rhodanobacter, Dokdonella and Rhodococcus were enhanced by ozone exposure. All the results verified that ozone injection is capable of sustaining the long-term performance of biofilters by lowering the biomass accumulation, increasing the microbial viability and changing the microbial community structure.

关键词： Biofilter Ozone VOCs Biomass control High-throughput sequencing

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