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Frontispiece: Recent Status and Developments of Vacancies Modulation in the ABO3Perovskites for Catalytic Applications

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Chemistry – A European Journal 2023年第8期29卷

作者： Dr. Jinxing Mi Dr. Jianjun Chen Xiaoping Chen Dr. Xiaoqing Liu Prof. Dr. Junhua Li State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 P. R. China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China School of Environment and Safety Engineering North University of China Taiyuan 030051 P. R. China

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Balancing Hydrogen Evolution and Hydrogenation Reaction via Facet Engineering for Efficient Conversion of Nitrate to Ammonia in Actual Wastewater

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Angewandte Chemie 2025年

作者： Wenye Zhong Prof. Yan Chen Peiyan Chen Qiaowen Chen Prof. Chunzhen Yang Prof. Nian Zhang Prof. Xueming Liu Prof. Zhang Lin School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling South China University of Technology Guangzhou 510006 China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution School of Metallurgy and Environment Central South University Changsha 410083 China School of Materials Sun Yat-Sen University Shenzhen 518107 China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China

Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution reaction (HER), the conventional approach to improve Faradaic efficiency is to select a catalyst without HER activity. Nevertheless, such a strategy not only limits the application of HER catalysts in NO 3 − RR, but also causes insufficient hydrogen source, thereby sacrificing ammonia yield rate. We believe that HER catalysts should not be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co 3 O 4 as model system, we reveal that the oxygen vacancies on crystal facet can greatly promote water dissociation and capture HER intermediate for NO 3 − RR, successfully shifting the reaction pathway from hydrogen evolution to nitrate hydrogenation. Beyond material development, we construct a hybrid reactor and achieve an ammonia recovery rate of 1216.8 g-N m −2 d −1 in nuclear industry wastewater with ultra-high nitrate concentration. This study breaks through the limitation of HER catalyst in NO 3 − RR, which provides a significant insight into the catalyst designing and hydrogenation mechanism.

关键词： Actual wastewater Ammonia recovery Coupling system Facet regulation Hydrogenation Oxygen vacancy Reactor designing

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Sustainable Synthesis of Concentrated Formate via CO2Electrolysis Integrated with Cl2Formation

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Angewandte Chemie 2025年

作者： Haocheng Xiong Donghuan Wu Runyu Jiang Haonan Li Qikun Hu Xi Lu Bingjun Xu Qi Lu State Key Laboratory of Chemical Engineering Department of Chemical Engineering Tsinghua University Beijing 100084 China College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Both authors equally contributed to this work. State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China Beijing Laboratory of Environmental Frontier Technologies Tsinghua University Beijing 100084 China Institute for Carbon Neutrality Tsinghua University Beijing 100084 China Ordos Laboratory Inner Mongolia 017000 China

Integrating CO 2 electrolysis with an industrially relevant anodic reaction enhances the economic feasibility and reduces carbon emissions in practical operations. In this study, we present an electrosynthesis strategy that integrates the CO 2 reduction reaction to produce concentrated formate solution with the Cl 2 formation in cation exchange membrane-based electrolyzers, scaling from 1 to 100 cm 2 electrode areas. Our process, equipped with two automated pH regulation strategies, achieved selectivities over 80% for formate and 95% for chlorine in a 25 cm 2 electrolyzer. Additionally, it demonstrated the ability to achieve formate concentrations up to 5.4 M during extended operation periods, establishing a new benchmark for electrochemical formate/formic acid synthesis. Techno-economic assessment and life cycle assessment further validated the process' sustainability, demonstrating a realistic path to profitability for valuable chemical production from CO 2 even without considering potential subsidies and carbon taxes.

关键词： Chlorine evolution reaction CO2 reduction reaction Life cycle assessment Process automation Techno-economic assessment

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Heteroaggregation of functionalized nanoplastics with Al 2 O 3 particles in aquatic environments

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Chemical Engineering Journal 2025年 518卷

作者： Xia Liu Yating Zhao Tongtao Yue Bo Gao Xing Guo Meng Wang Wenli Su Chu Wang Lu Liu Yanhui Dai Zhenyu Wang Jian Zhao Baoshan Xing Frontiers Science Center for Deep Ocean Multispheres and Earth System Institute of Coastal Environmental Pollution Control Key Laboratory of Marine Environment and Ecology (Ministry of Education) Ocean University of China Qingdao 266100 China Laboratory for Marine Ecology and Environmental Science Qingdao Marine Science and Technology Center Qingdao 266237 China State Key Laboratory of Simulation and Regulation of Water Cycle in River Basin China Institute of Water Resources and Hydropower Research Beijing 100038 China Institute of Environmental Processes and Pollution Control and School of Environment & Ecology Jiangnan University Wuxi 214122 China Stockbridge School of Agriculture University of Massachusetts Amherst MA 01003 United States

Heteroaggregation is critical for the distribution, transport, and bioavailability of nanoplastics in aquatic environments, but the heteroaggregation of functionalized nanoplastics with Al 2 O 3 particles is unknown. In this work, strong heteroaggregation occurred between negatively charged nanoplastics (PS-plain and PS-COOH) and positively charged Al 2 O 3 particles at pH 6.0, and electrostatic attraction was identified as the dominant force. Weak heteroaggregation was also found for positively charged PS-NH 2 , in which hydrogen bonding and van der Waals force were the main mechanism based on molecular dynamics simulations and Fourier transform infrared analysis. Maximum heteroaggregation rates and hydrodynamic diameters of PS-Al 2 O 3 heteroaggregates were observed at the ratio of 0.005 (PS-COOH/Al 2 O 3 ), which could be explained by the minimum net charge of the heteroaggregates in the binary system and the specific heteroaggregate configurations (bridging). Additionally, the effect of humic acid (HA) on PS-Al 2 O 3 heteroaggregation under different interaction sequences was studied for the first time. Notably, pre-treated with HA on PS-COOH nanoplastics or Al 2 O 3 mitigated the heteroaggregation more obviously relative to coating HA on PS-Al 2 O 3 heteroaggregates ((Al 2 O 3 -PS-COOH)-HA). Pre-adsorbed HA weakened electrostatic interaction and enhanced steric interactions between PS-COOH and Al 2 O 3 . For the three nanoplastics, homoaggregation of Al 2 O 3 facilitated PS-Al 2 O 3 heteroaggregation under low ionic strength (below 50 mM NaCl) while this effect was not evident under high ionic strength conditions. Slight disturbance (e.g., shaking) was found to enhance the heteroaggregation between PS nanoplastics and Al 2 O 3 , while strong disturbance (e.g., sonication) could break down PS-Al 2 O 3 heteroaggregates irreversibly. These results are useful for better understanding the transport and fate of nanoplastics in the natural aquatic environments.

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Corrigendum to "Mechanochemical destruction of perfluorooctane sulfonate (PFOS) using boron carbide (B4C)" [ J Hazard Mater 486 (2025) 137044]

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Journal of hazardous materials 2025年 485卷 137236页

作者： Lijie Duan Mengbin Gu Minghao Wang Liquan Liu Xue Cheng Xueqi Fan Jun Huang State Key Joint Laboratory of Environment Simulation and Pollution Control (SKLESP) Beijing China Key Laboratory for Emerging Organic Contaminants Control (BKLEOC) Beijing China Laboratory for Environmental Frontier Technologies (BLEFT) School of Environment Tsinghua University Beijing 100084 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing 100012 China. School of Environmental and Geographical Sciences Shanghai Normal University Shanghai 200234 China. China Metallurgical Industry Planning and Research Institute Beijing 100013 China. Laboratory for Environmental Frontier Technologies (BLEFT) School of Environment Tsinghua University Beijing 100084 China. Laboratory for Environmental Frontier Technologies (BLEFT) School of Environment Tsinghua University Beijing 100084 China. Electronic address: huangjun@***.

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Antagonism between ambient ozone increase and urbanization-oriented population migration on Chinese cardiopulmonary mortality

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The Innovation 2023年第6期4卷 48-58页

作者： Haitong Zhe Sun Junchao Zhao Xiang Liu Minghao Qiu Huizhong Shen Serge Guillas Chiara Giorio Zosia Staniaszek Pei Yu Michelle W.L.Wan Man Mei Chim Kim Robin van Daalen Yilin Li Zhenze Liu Mingtao Xia Shengxian Ke Haifan Zhao Haikun Wang Kebin He Huan Liu Yuming Guo Alexander T.Archibald lYusuf Hamied Department of Chemistry University of CambridgeCambridge CB21EWUK Department of Earth Sciences University of CambridgeCambridge CB23EQUK Department of Environmental Health and Engineering Johns Hopkins Bloomberg School of Public HealthBaltimoreMD 21205USA State Key Joint Laboratory of ESPC State Environmental Protection Key Laboratory of Sources and Control of Air Pollution ComplexSchool of EnvironmentTsinghua UniversityBejing 100084China School of Atmospheric Sciences Nanjing UniversityNanjing 210023China Department of Earth System Science Stanford UniversityStanfordCA 94305USA School of Environmental Science and Engineering Southern University of Science and TechnologyShenzhen 518p55China Department of Statistical Science University College LondonLondon WC1E 6BTUK The Alan Turing Institute London NW12DBUK School of Public Heath and Preventive Medicine Monash UniversityMelboumeVIC 3004Australia British Heart Foundation Cardiovascular Epidemiology Unit Department of Public Health and Primary CareUniversity of CambridgeCambridge CB18RNUK Heart and Lung Research Institute University of CambridgeCambridge CB20BDUK Baroelona Supercomputing Center Department of Earth Sciences08034 BarcelonaSpain School of Environmental Science and Engineering Nanjing University of Information Science and TechnologyNanjing 210044China Department of Mathematics University of CaliformiaLos AngelesLos AngelesCA 90095USA State Key Laboratory of New Ceramics and Fine Processing KeyLaboratory of Advanced Materials of Ministry of EducationSchool of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Department of Engineering University of CambridgeCambridge CB21PZUK National Centre for Atmospheric Science Cambridge CB21EWUK

Everincreasing ambient ozone(O3)pollution in China has been exacerbating cardiopulmonary premature ***,the urban-rural exposure inequity has seldom been ***,we assess populationcale 03 exposure and mortality burdens between 1990 and 2019 based on integrated pollution tracking and epidemiological *** find Chinese population have been suffering from climbing 03 exposure by 4.3±2.8 ppb per decade as a result of rapid urbanization and growing prosperity of socioeconomic *** residents are broadly exposed to 9.8±4.1 ppb higher ambient O3 than the adjacent urban citizens,and thus urbaniza-tion-oriented migration compromises the exposure-associated mortality on total *** excess premature deaths attributable to longterm 03 exposure,373,500(95%uncertainty interval[U]:240,600-510,900)in 2019,is underestimated in previous studies due to ignorance of cardiovascular *** 03 pollution policy should focus more on rural population who are facing an aggravating threat of mortality risks to ameliorate environmental health injustice.

关键词： ambient urban urbanization

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Dynamics of nitrogen oxides emissions in the pilot wastewater treatment plant: Characteristics and mechanisms

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Journal of environmental Sciences 2025年

作者： Xinyi Xu Ke Han Zhen Liu Huiqi Jiang Yanhui Zhao Jinhe Wang Jian Zhang Yangang Ren Zhen Hu School of Environmental Science & Engineering Shandong University Qingdao 266237 China Resources and Environment Research Institute School of Municipal and Environmental Engineering Shandong Jianzhu University Ji’nan 250101 China. State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China State Key Lab Microbial Technol Shandong University Qingdao 266237 China

Nitrogen oxides (NO x ), consisting of nitric oxide (NO) and nitrogen dioxide (NO 2 ), pose significant risks to human health and the environment, potentially causing respiratory and cardiovascular diseases. In contrast to extensive research on industrial NO x emissions, there has been a paucity of attention on the dynamics of NO x in wastewater treatment plants (WWTPs). This study investigated NO x emission patterns in a pilot-scale WWTP, revealing that NO dominated NO x emissions (0.013 % of the nitrogen load), peaking nocturnally (4 a.m.- 6 a.m.) and primarily originating from the oxic zone due to ammonia-oxidizing bacteria activity and aeration stripping synergistically increasing NO x emission. NO 2 emissions were minimal (0.003 % of the nitrogen load), with limited conversion from NO. Pearson correlation analysis identified ammonium removal efficiency and nitrate accumulation efficiency as key drivers of NO x production. The microbial community composition was closely linked to NO x emissions, with nitrifying bacteria such as Nitrosomonas contributing to NO x generation in the oxic zone, while denitrifying bacteria like Methylotenera contributed to NO x emissions under oxygen-limited conditions in the anoxic zone. This study enhanced the comprehension of the intricate processes of the nitrogen cycle during wastewater treatment and provided theoretical guidance for further optimization of WWTPs.

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Metabolic regulation of enhanced biodegradation of petroleum hydrocarbons through quorum sensing by extracellular metabolites of euglena

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Journal of Hazardous Materials 2025年

作者： Guotao Chen Meng Yuan Guanghong Xie Yibo Xiao Yujiao Qu Yuan Ren School of Environment and Energy South China University of Technology Guangzhou 510006 PR China Protoga Biotechnology Co. Ltd. Shenzhen 518000 China Microalgae Biosynthesis R&D Center Research Institute of Tsinghua University in Shenzhen Shenzhen 518057 China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of Education PR China The Key Laboratory of Environmental Protection and Eco-Remediation of Guangdong Regular Higher Education Institutions PR China

The quorum sensing (QS) system can regulate and enhance the degradation of petroleum pollutants. Enhancing the indigenous microbial QS system by adding environmentally friendly biostimulants is currently a preferred strategy for achieving high stability, sustainability, and cost-effective biodegradation of petroleum contaminants. However, the intrinsic mechanisms by which biostimulants induce QS-mediated regulation of petroleum hydrocarbon degradation remain unclear. Unlike traditional QS regulation strategies, the aim of this study was to explore the mechanisms of the extracellular metabolites of euglena (EME) stimulant to enhance the degradation of diesel by Pseudomonas aeruginosa LNR1 through QS inhibitor (eugenol) damaging QS system. Results showed that the addition of eugenol reduced the degradation rate of diesel, down-regulated the expression of degradation-related hydroxylation and dehydrogenation genes, and inhibited the synthesis of extracellular polymer (EPS) and biofilm. Further, we found that that eugenol reduced the intracellular synthesis of three signal molecules (C4-HSL, 3-oxo-C12-HSL, and PQS) of Pseudomonas aeruginosa , among which 3-oxo-C12-HSL showed obvious intracellular accumulation. The genes of the three signaling molecules synthesis and the 3-oxo-C12-HSL transport system (MexAB-OprM) were down-regulated. Eugenol had a strong affinity with the peripheral plasma membrane fusion protein (MexA) of the 3-oxo-C12-HSL transport system, and the transport function was obviously inhibited. Eugenol also has hydrogen bond interaction with translocase and receptor protein of signal transduction that regulate signal transduction. The above results indicated that the biostimulant controlled the QS system by inducing microorganisms to change the synthesis, transport and signal transduction of signal molecules, thus affecting metabolic functions related to degradation and promoting the degradation of pollutants.

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Synergistic effect of cobalt iron layered double hydroxides with adjacent copper atoms regulates intermediate adsorption and H 2 O dissociation to boost electrocatalytic nitrate reduction at ultralow concentrations

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Applied Catalysis B: environment and Energy 2025年 378卷

作者： Mingming Zhang Cui Lai Bisheng Li Fuhang Xu Xiaorui Hu Dengsheng Ma Lin Tang College of Environmental Science and Engineering Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University) Ministry of Education Changsha Hunan 410082 PR China Institute of Environment and Ecology Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 PR China College of Geography and Environmental Sciences Zhejiang Normal University Jinhua Zhejiang 321004 PR China

Electrocatalytic nitrate reduction to ammonia is a promising strategy for removing contaminated nitrate in wastewater and simultaneously generating ammonia. Herein, cobalt iron layered double hydroxides modified Cu foam (Co 2.76 Fe LDH/Cu) as dual-active sites tandem catalysts was synthesized for electrocatalytic nitrate reduction. Co 2.76 Fe LDH/Cu exhibits high selective nitrate conversion to ammonia in a broad concentration window (1–100 mM). Especially, the high Faradaic efficiency (94.50 %) and ammonia generation (2.16 mg h −1 cm −2 ) in ultralow nitrate concentrations (1 mM) was obtained at −0.54 V. In-situ Raman reveals the tandem catalytic mechanism, in which Cu phases catalyze reduction NO 3 - to highly oxidative NO 2 , and Co 2.76 Fe LDH phases is locally oxidized and provides sufficient electrons to promote NO 2 - -to-NH 3 conversion. Meanwhile, theoretical calculations also reveal that NO 3 - -to- NO 2 - conversion occurs at the Cu site of Co 2.76 Fe LDH/Cu, and the introduction of Fe can increase the thermodynamic favorability of NO 2 - adsorption. In-situ Fourier transform infrared spectra, theoretical calculations, and electron spin resonance show the strong H 2 O dissociation during NO 3 - RR process, which can provide abundant active hydrogen (*H) species for the intermediates hydrogenation and ultimately improve ammonia generation.

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Coupling of the galvanic cell and Z-scheme effects of zinc/gallium dual co-catalysts to enhance the photocatalytic conversion of carbon dioxide using water as an electron donor

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Journal of environmental Sciences 2025年

作者： Xuanwen Xu Shuying Wang Ying Luo Pengyu Dong Pengyu Wu Zheng Wang Ruiyu Jiang Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province Yancheng Institute of Technology Yancheng 224051 China School of Chemistry and Chemical Engineering Yancheng Institute of Technology Yancheng 224051 China School of Mechanics and Safety Engineering Zhengzhou University Zhengzhou 450001 China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China College of Resources and environment University of the Chinese Academy of Sciences Beijing 101408 China

Zinc/gallium (Zn/Ga) dual co-catalysts consisting of Zn 0 and amorphous ZnGa 2 O 4 species were found to selectively produce carbon monoxide (CO) during the photocatalytic conversion of carbon dioxide (CO 2 ) using water (H 2 O) as an electron donor over photocatalysts such as NaTaO 3 , Ga 2 O 3 , and ZnGa 2 O 4 , and in the electrochemical reduction of CO 2 over Zn 0 electrodes. It is considered that there are two effects associated with the Zn/Ga dual co-catalysts: (1) A galvanic cell effect between Zn 0 and amorphous ZnGa 2 O 4 , and (2) a Z-scheme effect in NaTaO 3 /Zn 0 /amorphous ZnGa 2 O 4 . The coupling of these two effects favored the active and selective evolution of CO during the photocatalytic conversion of CO 2 by H 2 O.

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