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Enhanced Ru–Ce interface electron transfer and reverse oxygen spillover promote chlorobenzene catalytic oxidation

Applied Catalysis B: environmental 2025年 373卷

作者： Chen, Deli Si, Wenzhe Wang, Rong Yuan, Xing Zhou, Bin Chen, Zhen Peng, Yue Li, Junhua State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China

The catalytic oxidation of chlorinated volatile organic compounds (CVOCs) is still a big challenge due to chlorine poisoning and the polychlorinated byproducts. Ru-loaded CeO2 catalysts have attracted much attention in CVOCs oxidation. To optimize the surface electronic structure of Ru/CeO2, we reduced the CeO2 support to enhance the metal-support interaction of the Ru/CeO2 catalyst, resulting in higher Ru dispersion and stronger interface electron transfer. The Reduction treatment not only enhances the activation of O2 molecules by promoting the generation of interface electron-rich units but also stimulates stronger reverse oxygen spillover (ROS). The improved oxygen activation and migration ability accelerates the decomposition of intermediate products. Besides, the lower surface electrostatic potential also weakens the chlorine adsorption of the catalyst. After the modification, the oxidation rate of chlorobenzene increased by more than 1.5 times at 240–320 °C and the T90 decreased by about 50 °C. © 2025

关键词： Catalytic oxidation

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Machine learning for membrane bioreactor research:principles,methods,applications,and a tutorial

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Frontiers of environmental Science & Engineering 2025年第3期19卷 119-144页

作者： Yizhe Lai Kang Xiao Yifan He Xian Liu Jihua Tan Wenchao Xue Aiqian Zhang Xia Huang Beijing Yanshan Earth Critical Zone National Research Station College of Resources and EnvironmentUniversity of Chinese Academy of SciencesBeijing 101408China Key Laboratory of Earth System Numerical Modeling and Application University of Chinese Academy of SciencesBeijing 101408China Environmental Chemistry Faculty College of Resources and EnvironmentUniversity of Chinese Academy of SciencesBeijing 101408China State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Department of Energy Environmentand Climate ChangeSchool of EnvironmentResourcesand DevelopmentAsian Institute of TechnologyP.O.Box 4Klong LuangPathumthani 12120Thailand State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

Membrane fouling poses a significant challenge to the sustainable development of membrane bioreactor(MBR)technologies for wastewater *** accurate prediction of the membrane filtration process is of great importance for identifying and controlling *** learning methods address the limitations of traditional statistical approaches,such as low accuracy,poor generalization ability,and slow convergence,particularly in predicting complex filtration and fouling processes within the realm of big *** article provides an in-depth exposition of machine learning *** study then reviews advances in MBRs that utilize machine learning methods,including artificial neural networks(ANN),support vector machines(SVM),decision trees,and ensemble *** on current literature,this study summarizes and compares the model input and output characteristics(including foulant characteristics,solution environments,filtration conditions,operating conditions,and time factors),as well as the selection of models and optimization *** modeling procedures of SVM,random forest(RF),back propagation neural network(BPNN),long short-term memory(LSTM),and genetic algorithm-back propagation(GA-BP)methods are elucidated through a tutorial *** simulation results demonstrated that all five methods yielded accurate predictions with R2>***,the existing challenges in the implementation of machine learning models in MBRs were *** is notable that integration of deep learning,automated machine learning(AutoML)and explainable artificial intelligence(XAI)may facilitate the deployment of models in practical engineering *** insights presented here are expected to facilitate the establishment of an intelligent control framework for MBR processes in future endeavors.

关键词： Membrane bioreactor Machine learning Pollutant removal Membrane fouling Model prediction

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Remarkable Enhancement of the Activity and Hydrothermal Stability of a CeO2-Based NH3-SCR Catalyst by Sn Modification

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Engineering 2025年 48卷 141-150页

作者： Zhu, Ying Liu, Jingjing He, Guangzhi Xie, Shaohua Shan, Wenpo Lian, Zhihua Liu, Fudong He, Hong Center for Excellence in Regional Atmospheric Environment & Key Laboratory of Urban Pollutant Conversion Institute of Urban Environment Chinese Academy of Sciences Xiamen361021 China Zhejiang Key Laboratory of Pollution Control for Port-Petrochemical Industry Ningbo Urban Environment Observation and Research Station Institute of Urban Environment Chinese Academy of Sciences Ningbo315800 China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing100085 China University of Chinese Academy of Sciences Beijing100049 China Department of Civil Environmental and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations NanoScience Technology Center University of Central Florida OrlandoFL32816 United States

Catalytic activity and hydrothermal stability are both crucial for the application of the selective catalytic reduction of NOx with NH3 (NH3-SCR) catalyst in diesel vehicles. In this study, a tin (Sn)-modified Ce–Nb mixed-oxide catalyst was synthesized as an NH3-SCR catalyst for NOx emission control. After the introduction of Sn, both the NH3-SCR activity and the hydrothermal stability of the catalyst were remarkably promoted. Even after hydrothermal aging at 1000 °C, the developed Ce1Sn2Nb1Ox catalyst achieved more than 90% NOx conversion at 325–500 °C. Various methods, including N2-physisorption, X-ray diffraction, in-situ high-temperature X-ray diffraction, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray absorption fine-structure spectroscopy, temperature-programmed reduction of hydrogen, temperature-programmed desorption of ammonia, and density functional theory calculations were used to investigate the promotional effects induced by the Sn species. The characterization results showed that the addition of Sn not only promoted the formation of the Ce–Nb active phase but also improved its thermal stability, contributing to the excellent NH3-SCR performance and hydrothermal stability. This study provides an excellent sintering-resistance catalyst for the application of diesel engine NOx emission control. © 2025 THE AUTHORS

关键词： Temperature programmed desorption

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Forest Mercury Deposition Observation in Chongqing: Evaluating Effectiveness of Mercury pollution control over the Past Decade in Southwestern China

ACS ES&T Air

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ACS ES&T Air 2025年第2期2卷 286-294页

作者： Ziyi Zhan Dongwei Lv Huang Zhou Qingru Wu Yuying Cui Lei Duan State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University 100084 Beijing China School of the Environment Nanjing University 210023 Nanjing China State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University 100084 Beijing China；State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Tsinghua University 100084 Beijing China

As the largest Hg reservoir in terrestrial ecosystems, forests provide valuable insights into atmospheric Hg levels through observations of mercury deposition. In this study, we conducted a one-year observation of Hg deposition, by both throughfall and litterfall, in a forest located in Chongqing, an industrial hub in southwestern China, in 2021. We compared the results with observations made at the same sampling site in 2010–2011. The results showed that there were significant decreases in both Hg concentrations (from 115 μg·kg–1to 80.2 μg·kg–1for litterfall and from 68.4 ng·L–1to 4.01 ± 2.09 ng·L–1for throughfall) and Hg deposition fluxes (from 89.8 μg·m–2·yr–1to 19.9 μg·m–2·yr–1for total deposition, decreasing by 77.8%) in the forest from 2010 to 2021. The decrease in deposition might result from the synergistic effect of reduction in both anthropogenic (inventory-listed or nonquantitative) and re-emission sources. Over the decade since the initiation of theMinamata Convention on Mercury, atmospheric Hg levels have decreased significantly, mainly due to the co-benefits of conventional air pollutant control, indicating the effectiveness of China’s Hg pollution control policies.

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Simultaneous removal of NH4+ and NO3– by coupling sulfur-based autotrophic denitrification and ANAMMOX with different electron donors

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Separation and Purification Technology 2025年 363卷

作者： Zhu, Liang Chen, Zhiqiang Wen, Qinxue Huang, Xia State Key Laboratory of Urban Water Resource and Environment School of Environment Harbin Institute of Technology Harbin150090 China State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China

Unstable nitrite supply and low ammonia concentration limited the application of mainstream Anammox. In this study, sulfur-based autotrophic denitrification coupled Anammox system (SADA) was established with pyrite and sulfur as electron donors, respectively, to simultaneously remove NH4+-N and NO3–-N. More than 85 % of the total inorganic nitrogen removal efficiency was achieved with S0 as the electron donor. The synergistic nitrogen removal of autotrophic denitrification and Anammox reduced SO42− production. The average NH4+-N removal efficiency reached 94.73 % when pyrite was used as the electron donor, but the NO3–-N concentration in the effluent was higher than that in the influent. Microorganisms associated with nitrogen cycle were significantly enriched at the bottom of both reactors, where major biochemical processes occurred. Batch tests showed the coexistence of multiple N metabolic pathways in SADA, including Anammox, autotrophic denitrification, Sulfammox and Feammox. The genus Thiobacillus, Ferritrophicum, Candidatus_Brocadia, Ignavibacterium and Thermoanaerobaculum played major roles in nitrogen removal. © 2025

关键词： Denitrification

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Optimization on the Preparation Conditions of Fe-N/BC Catalyst and its pollution Removal Efficiency 6

Optimization on the Preparation Conditions of Fe-N/BC Cataly...

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2024 6th International Conference on Advanced Materials and Ecological environment, AMEE 2024

作者： Zhou, Ting Yang, Yang Du, Tianxing Dong, Wenyi Wang, Hongjie School of Civil and Environmental Engineering Harbin Institute of Technology Shenzhen Guangdong Shenzhen518055 China Shenzhen Key Laboratory of Water Resource Utilization and Environmental Pollution Control Guangdong Shenzhen518055 China State Key Laboratory of Urban Water Resource and Environment School of Environment Harbin Institute of Technology Heilongjiang Harbin150090 China

This study was aimed to optimize the preparation conditions of Fe-N/BC catalyst. Citric acid iron and melamine was used to co-doped modified selected biomass, optimized factors included biomass type, acid washing time, iron-nitrogen doping amount and pyrolysis temperature, with nitrobenzene as the targeted degradation object. The optimal preparation conditions for Fe-N/BC iron-nitrogen co-doped biochar catalyst were determined. The results showed that using onion as the biomass, after 8 hours of acid washing, immersed in an ultrasonic solution of citric acid iron with a concentration of 8 g/L for 30 minutes, followed by adding melamine at a doping ratio of 5 g/g biomass and another 30 minutes of ultrasonication, centrifuged, water washed, and dried, then pyrolyzed at 900°C under N2 atmosphere for 1 hour. The obtained Fe-N/BC iron-nitrogen co-doped biochar catalyst exhibited the best removal efficiency for nitrobenzene in a catalytic reduction system, with a removal rate of 96.6% after 15 minutes of reaction. © Published under licence by IOP Publishing Ltd.

关键词： Semiconductor doping

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Study on the Morphological Structure Characteristics of the Modified Preparation Fe-N/BC Catalysts 6

Study on the Morphological Structure Characteristics of the ...

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2024 6th International Conference on Advanced Materials and Ecological environment, AMEE 2024

作者： Yang, Yang Zhou, Ting Du, Tianxing Dong, Wenyi Wang, Hongjie School of Civil and Environmental Engineering Harbin Institute of Technology Shenzhen Guangdong Shenzhen518055 China Shenzhen Key Laboratory of Water Resource Utilization and Environmental Pollution Control Guangdong Shenzhen518055 China State Key Laboratory of Urban Water Resource and Environment School of Environment Harbin Institute of Technology Heilongjiang Harbin150090 China

In this study, the citric acid iron and melamine was used to modify the selected biomass, preparing Fe-N/BC iron-nitrogen co-doped biochar catalyst. The BC, N/BC, and Fe-N/BC were characterized by SEM, XRD, FTIR, Raman, XPS, etc., to research the aspects of micromorphology, crystal structure, surface functional group types, and element composition. The results showed that Fe and N elements could be doped into the biochar successfully, making the particle size of Fe-N/BC smaller than that of BC, possessing a bigger surface area with a more abundant pore structure. Additionally, the graphitization degree of Fe-N/BC was enhanced, introducing active sites including pyridinic nitrogen, graphitic nitrogen, and Fe-Nx, enhancing the catalytic activity and electron transfer performance of the catalyst, enabling Fe-N/BC to simultaneously act on catalytic reduction and catalytic oxidation systems. © Published under licence by IOP Publishing Ltd.

关键词： Catalytic oxidation

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Degradation Kinetics of Nitrobenzene and Aniline by Fe-N/BC Redox System 6

Degradation Kinetics of Nitrobenzene and Aniline by Fe-N/BC ...

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2024 6th International Conference on Advanced Materials and Ecological environment, AMEE 2024

This study was aimed to analysis the degradation kinetics of nitrobenzene and aniline by the Fe-N/BC redox system. Factors such as the initial pH of the solution, PMS/NaBH4 concentrations, and pollutant concentrations were investigated to explore the variations in pollutant degradation rates in the system. The results indicated that the Fe-N/BC-catalyzed NaBH4 reduction of nitrobenzene followed first-order kinetics, while the Fe-N/BC-catalyzed PMS oxidation of aniline followed pseudo-first-order kinetics. When the pH was alkaline, the reaction was inhibited. Increasing the addition of NaBH4 and PMS from 0.05 to 0.5 g/L resulted in the reaction rate constants for nitrobenzene and aniline increasing from 0.115, 0.120 min-1 to 0.743, 0.354 min-1, respectively. As the pollutant concentration gradually rose from 2 to 50 mg/L, the reactions were inhibited, with the reaction kinetics for nitrobenzene and aniline decreasing from 0.348, 0.288 min-1 to 0.147, 0.091 min-1, respectively. © Published under licence by IOP Publishing Ltd.

关键词： Nitrobenzene

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Significant changes in the physicochemical properties of BC-containing particles during the cold season in Beijing

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Journal of environmental Sciences 2025年第5期151卷 667-676页

作者： Shuya Hu Linghan Zeng Gang Zhao Shiyi Chen Chunsheng Zhao Weilun Zhao Min Hu State Key Joint Laboratory of Environmental Simulation and Pollution Control International Joint Research Center for Atmospheric Research(IJRC)College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Department of Atmospheric and Oceanic Sciences School of PhysicsPeking UniversityBeijing 100871China Collaborative Innovation Center of Atmospheric Environment and Equipment Technology Nanjing University of Information Science and TechnologyNanjing 210044China

The ambient air quality has improved significantly under strict emission controls in Beijing,China over the last *** carbon(BC),as a short-lived climate forcer in ambient aerosols,profoundly impacts the air quality and *** studies have demonstrated a decline in the mass concentration of *** this study,we characterized the chemical compositions and size distributions of BC-containing particles during the cold season of 2022 in Beijing using state-of-the-art instruments capable of exclusively measuring BCcontaining *** optical properties of BC-containing particles were further calculated based on the Mie ***,we compared the properties of BC-containing particles in 2022 with the results of previous *** results showed that the diameters of BC cores became larger while the coating thickness of BC-containing particles became thinner in *** the coating materials,the mass fraction of nitrate increased obviously,and even replaced organic matter as the dominant component during the peak of the pollution *** in chemical compositions and size distributions resulted in lower mass absorption cross-sections(MAC)of BC-containing particles from 10.5±1.1 m^(2)/g in 2016 to 7.3±0.8 m^(2)/g in 2022,reduced by 30.5%.Our results demonstrate the synergistic benefits of air pollution control in improving air quality and mitigating climate ***,the MAC of BC adopted in climate models should vary with the changing air pollution *** study emphasizes that it is imperative to conduct long-term observations of BC-containing particles to better estimate BC’s climate effects.

关键词： Black carbon Chemical composition Size distribution Light absorption ability

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Seasonal changes of chemodiversity along with microbial succession in a municipal wastewater treatment plant

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Journal of environmental Sciences 2025年第4期150卷 318-331页

作者： Yunwei Cui Junya Zhang Luoyao Wen Jibao Liu Zhineng Hao Chunzhong Wei Yanbo Jiang Yuansong Wei Peihong Shen College of Life Science and Technology Guangxi UniversityNanning 530005China State Key Joint Laboratory of Environmental Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Guangxi Beitou Environmental Protection&Water Group Co. LTD.Nanning 530025China

The relationship between chemodiversity and microbial succession in wastewater treatment plants(WWTPs)is highly intricate and *** specific contribution of the microbial community to changes in the composition of dissolved organic matter(DOM)within different biological treatment units remains unclear,as does the reciprocal influence of DOM composition on microbial *** this study,spectroscopy((Excitationemission matrix)EEM-PARAFAC,Ultraviolet(UV)-spectrum,Fourier transform infrared spectrometer(FT-IR)),Liquid chromatograph mass spectrometer(LC–MS)and Fourier transform ion cyclotron resonance(FT-ICR)MS along with high-throughput sequencing technology were used to explore the relationship between chemodiversity and microbial succession in WWTPs concerning seasonal *** results showed that WWTPs with anaerobic/anoxic/oxic(A2O)processes can metabolize and transformmost of thewastewater DOM,and the anaerobic unit has the highest removal rate for fluorescence DOM(FDOM,14.07%-64.43%);the anaerobic unit increased aliphatic/proteins and lignin-like molecules but decreased relative intensity,while the anoxic unit removed unsaturated hydrocarbons,aromatic structures,and lignin-like *** impact of seasonal changes on the composition and removal of FDOM and DOM in wastewater treatment is significant,and the variations that occur during different seasons affect microbial activity,as well as the production,degradation,and transformation of organic compounds throughout thewastewater treatment *** analysis shows that Parcubacteria_genera_incertae_sedis plays a crucial role in DOM chemodiversity,highlighting the crucial contribution of microbial com-munities to both the structure and operation of the entire DOM *** results in this study could provide some theoretical and practical basis for guiding the process optimiza-tion of WWTPs.

关键词： Wastewater treatment plant Dissolved organic matter Fourier transform ion cyclotron resonance mass spectrometry Chemodiversity Microbial community

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