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Selective polymerization of chlorophenols in hypersaline wastewater via surface-complex-mediated electron transfer over Ce-doped CuO

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Water Research 2025年

作者： Wenjing Xie Zhenxin Wang Yifan Yin Yibo Bai Jiaqi Yang Delu Miao Xiangkang Zeng Shengjiong Yang Gen Wang Shaanxi Key Laboratory of Environmental Engineering School of Environmental and Municipal Engineering Xi’an University of Architecture and Technology Xi’an Shaanxi 710055 China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Petroleum Molecular & Process Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Dow Centre for Sustainable Engineering Innovation School of Chemical Engineering The University of Queensland St Lucia Queensland 4072 Australia

Conventional radical-based advanced oxidation processes (AOPs) for chlorophenol (CP) removal in hypersaline wastewater face critical challenges, including excessive oxidant demand, rapid radical quenching by chloride ions, and toxic chlorinated byproduct formation. Here, we report a nonradical electron transfer (ETP)-driven polymerization strategy that enables complete CP elimination without mineralization. By employing cerium-doped mesoporous CuO (Ce-CuO) with peroxydisulfate (PDS), 4-chlorophenol (4-CP) was selectively oxidized into phenoxy radicals via a surface-activated Ce-CuO@PDS complex, followed by polymerization into insoluble solid organic polymers. At a low PDS dosage (1.0 mM), 100% 4-CP (0.78 mM) removal was achieved with 86.4% total organic carbon (TOC) conversion to polymers. Mechanistic studies confirmed ETP dominance over radical pathways, with interfacial oxygen vacancies (Cu + -Ov-Ce 3+ ) reducing PDS adsorption energy ( vs . pristine CuO) and enhancing electron transfer efficiency. The strategy demonstrated robust performance under hypersaline conditions (Cl − , 3000-10000 mg L −1 ) and superior selectivity when treating paper mill wastewater. Notably, the system achieved a high decontamination capacity (3.74 g 4-CP per gram catalyst) while consuming 89% less oxidant than mineralization-based methods. This work establishes a sustainable paradigm for treating refractory organics in high-salinity industrial effluents through ETP-driven polymerization.

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Simulation of Thermal Wake in Conjugate Heat Transfer between a Sphere and its Surrounding Fluid

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SSRN 2022年

作者： Zhang, Nan Sun, Li Liu, Jufang Liu, Xinhua State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing100049 China Innovation Academy for Green Manufacture Chinese Academy of Sciences Beijing100190 China State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing102249 China

Unsteady conjugate heat transfer between a sphere and its surrounding water was investigated by 3D CFD simulations. The fluid flow was considered viscous and incompressible, the sphere region was set as solid, and the energy equations in the fluid and solid regions were solved numerically. The effect of Re numbers on local heat transfer and especially the thermal wake phenomenon was analyzed and Re = 8000 is determined as the turning point that thermal wake disappears. Two modes of reverse heat transfer, laminar and vortical were identified according to the starting position of the thermal inversion point, and the compromise of the convective and diffusive heat transfer mechanism was discussed. © 2022, The Authors. All rights reserved.

关键词： Spheres

Constructing Multilevel Structure with Microdomains of Oxides on Three-Dimensional High-Entropy Alloy Support Toward Efficient Oxygen Evolution

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SSRN 2022年

作者： Zhang, Shaofei Guo, Jing Li, Tiantian Sun, Jinfeng Meng, Yongqiang Kang, Jianli Tan, Linli Zhang, Zhijia Hebei Key Laboratory of Flexible Functional Materials Hebei Key Laboratory of Material Near-Net Forming Technology School of Materials Science and Engineering Hebei University of Science and Technology Shijiazhuang050018 China Key laboratory of Advanced Ceramics and Machining Technology Ministry of Education School of Materials Science and Engineering Tianjin University Tianjin300072 China Key Laboratory of Green Manufacturing of Super-light Elastomer Materials of State Ethnic Affairs Commission College of Intelligent systems Science and Technology Hubei Minzu University Enshi445000 China State Key Laboratory of Separation Membrane and Membrane Process Tianjin Municipal Key Laboratory of Advanced Fibers and Energy Storage School of Materials Science and Engineering Tiangong University Tianjin300387 China

High-entropy alloys (HEAs) with maximized configurational entropy has shown a great promise for anodic water splitting, but still limited to their unsatisfactory configuration and large-scaled application. In the present study, a series of dual-phase electrodes with spinel MnCr2O4 microdomains pinning on large-scaled and flexible surface oxidized high-entropy alloys (O-HEA) as highly efficient electrocatalysts is prepared by combining modified non-solvent induced phase separation (NIPs) and metallurgy approaches. The precipitation of MnCr2O4 microdomains from O-HEA support not only result in a shrinking of lattice constant of HEA but also lead to a surface reconstruction. Besides, the MnCr2O4 microdomains can synergy with reconstructed O-HEA support to increase the hydrophilic property and provide high-efficient electron/ion transport, thus promoting the O-O coupling. By virtues of the multilevel structure, the O-HEA2 electrode exhibits impressive oxygen evolution properties with a low overpotential of 268 mV and Tafel slope of 51.6 mV dec−1 in 1M KOH at 10 mA cm−2. It also exhibits a long durability exceed 70 h at 25 mA cm−2. This work provides a new prospect for the rational design of large-scaled and self-supported 3D HEA based electrodes for energy conversion applications. © 2022, The Authors. All rights reserved.

关键词： Catalyst activity

High load mixed matrix membrane by metal-organic polyhedra for enhanced gas separation

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Journal of Membrane Science 2025年 733卷

作者： Ju Bai Luqi Xiao Hongyan Liu Can Wang Tianliang Han Lili Gong Shuangjiang Luo Hongwei Fan Linglong Shan Chengdu Institute of Organic Chemistry Chinese Academy of Sciences Chengdu 610041 PR China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Beijing Key Laboratory of Solid State Battery and Energy Storage Process Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 PR China University of Chinese Academy of Sciences Beijing 100049 PR China The State Key Laboratory of Chemical Resource Engineering College of Chemical Engineering Beijing University of Chemical Technology Beijing 100029 PR China

Mixed matrix membranes (MMMs) are emerging as a competitive option in gas separation owing to their ability to mitigate the trade-off. Metal-organic polyhedra (MOPs) are a family of self-assembled structures consisting of metal ions and ligands, which are nanoscale cage-like molecules with independent units and excellent dispersion properties, while maintaining the similar pore structure of metal-organic frameworks (MOFs). Herein, Zr-MOP was incorporated as a filler in polybenzimidazole (OPBI) to achieve a high MOP loading of 50 wt%. The membrane with highly dispersed MOPs effectively prevents the excessive collaps of OPBI under the thermal treatment at 600 °C. The synergistic combination of Zr-MOP and OPBI yields perfectly dense, defect-free membranes with uniform pores and superior gas molecular selectivity. The optimal Zr-MOP 50 wt% @OPBI 600 membrane exhibited a remarkable He/CH 4 selectivity of 785, which is 4 times higher than the pristine OPBI membrane, alongside a high He permeability of 147 Barrer. Furthermore, the membrane demonstrated excellent high-pressure stability and long-term durability.

关键词： Oxygen permeable membranes

The application of molecular simulation in ash chemistry of coal

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Chinese Journal of Chemical engineering 2020年第11期28卷 2723-2732页

作者： Xin Dai Jin Bai Ping Yuan Shiyu Du Dongtao Li XiaodongWen Wen Li Beijing Key Laboratory of Green Recyclable Process for Iron&Steel Production Technology Beijing 100043China Shougang Group Research Institute of Technology Beijing 100043China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuan 030032China Engineering Laboratory of Specialty Fibers and Nuclear Materials Institute ofMaterial TechnologiesNingbo Institute ofMaterials Technology&EngineeringChinese Academy of SciencesNingbo 315000China

One of the crucial issues in modern ash chemistry is the realization of efficient and clean coal ***,large-scale coal gasification technology is well known as the foundation to improve the atom *** practice,the coal ash fusibility is a critical factor to determine steady operation standards of the gasifier,which is also the significant criterion to coal species selection for *** coal behaviors are resultant from various evolutions in different scales,the multi-scale understanding of the ash chemistry is of significance to guide the fusibility adjustment for coal *** important roles of molecular simulation in exploring ash chemistry,this paper reviews the recent studies and developments on modeling of molecular systems for fusibility related ash chemistry for the first *** discussions are emphasized on those performed by quantum mechanics and molecular mechanics,the two major simulation methods for microscopic systems,which may provide various insights into fusibility *** review article is expected to present comprehensive information for recent molecular simulations of coal chemistry so that new clues to find strategies controlling the ash fusion behavior can be obtained.

关键词： Coal ash Fusibility Molecular simulation Quantum mechanics Ash fusion temperature Viscosity

Insights into Enhanced Toluene Oxidation Performance Over Mn-Mof-Derived Catalysts Via Isogenous Ionic Surface Doping

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SSRN 2023年

作者： Wang, Jianshen Zhang, Di Zhao, Gangguo Yuan, Hua Liu, Dan Kuvarega, Alex T. Mamba, Bhekie B. Li, Hu Gui, Jianzhou State Key Laboratory of Separation Membranes and Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process Engineering School of Material Science and Engineering Tiangong University Tianjin300387 China School of Chemical Engineering and Technology Tiangong University Tianjin300387 China School of Chemistry Tiangong University Tianjin300387 China Ningxia Coal Industry Co. Ltd. Chn Energy Yinchuan750011 China Institute for Nanotechnology and Water Sustainability College of Science Engineering and Technology University of South Africa Florida Johannesburg1709 South Africa

A series of MnOx catalysts were prepared through a Mn-MOF-derived method, and their phase structures gradually change from Mn3O4-Mn2O3 to Mn2+ doped Mn2O3, and finally to Mn2O3 with increasing calcination temperature. The optimum MnOx-500 catalyst calcined at 500ºC, in the form of Mn2+-doped-Mn2O3 phase was used to construct an isogenous ion surface doped catalyst, which exhibited the best catalytic performance for toluene oxidation due to the large average pore size, the enhanced low-temperature redox properties, weakest Mn-O bond and the highest percentage of low-valence Mn(II) species. The possible route of toluene oxidation was proposed based on in-situ FTIR, and interestingly all the reaction intermediates including benzyl, benzyl alcohol, benzaldehyde, benzoate, phenol, maleate and formate, were produced on MnOx-400;while for MnOx-500, Mn2+-doped-Mn2O3, only benzyl, benzaldehyde, benzoate, maleate and formate were formed, and the rate-determining step for conversion of benzoate into ring-oping products requires less energy. The work opens a new avenue to the precise construction of active sites based on multivalent metal oxide catalysts for dehgradation of volatile organic compounds. © 2023, The Authors. All rights reserved.

关键词： Pore structure

Highly active N,O-doped hierarchical porous carbons for high-energy supercapacitors

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Chinese Chemical Letters 2020年第5期31卷 1226-1230页

作者： Ziyang Zhou Hui Duan Zhiwei Wang Yaokang Lv Wei Xiong Dazhang Zhu Liangchun Li Mingxian Liu Lihua Gan Shanghai Key Lab.of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China State Key Laboratory of Pollution Control and Resources Reuse Shanghai Institute of Pollution Control and Ecological SecuritySchool of Environmental Science and EngineeringTongji UniversityShanghai 200092China College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310014China School of Chemistry and Environmental Engineering Key Laboratory for Green Chemical Process(Ministry of Education)Hubei Key Lab.of Novel Reactor&Green Chemical TechnologyWuhan Institute of TechnologyZhengzhou 450001China College of Chemistry and Molecular Engineering Zhengzhou UniversityWuhan 430205China

Highly active N,O-doped hierarchical porous carbons(NOCs)are fabricated through the in-situ polymerization and pyrolysis of o-tolidine and ***-prepared NOCs have a variety of faradaic-active species(N-6,N-5 and O-I),high ion-accessible platform(1799 m^2/g)and hierarchically micro-meso-macro porous ***,the resultant NOC electrode delivers an advantageous specific capacitance(311 F/g),with a pseudocapacitive contribution of 37%in a threeelectrode configuration,and an enhanced energy output of 18.0 Wh/kg@350 W/kg owing to the enlarged faradaic effect in an aqueous redox-active ***,a competitive energy density(74.9 Wh/kg)and high-potential durability(87.8%)are achieved in an ionic liquid(EMIMB F4)-assembled *** study sheds light on a straightforward avenue to optimize the faradaic activity and nanoarchitecture for advanced supercapacitors.

关键词： N.O-doped carbon Hierarchical porous structure Faradaic activity Supcrcapacitor High energy density

Electrochemical behaviors of anode materials and their performance for bauxite desulfurization

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Chinese Journal of Chemical engineering 2019年第4期27卷 802-810页

作者： Yingnan Hu Aijing Lü Mingyong Wang Dong Wang Junhao Liu Zhi Wang Xuzhong Gong National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China State Key Laboratory of Advanced Metallurgy University of Science and Technology Beijing Beijing 100083 China

Pyrite inside bauxite could be oxidized into soluble S-containing ions by electrolysis, and thus achieving bauxite desulfurization by using filtration. However, S-containing ions in electrolyte had some corrosion effects on electrode, especially for anode. In this work, six kinds of traditional materials were selected as anode, and their corrosion behaviors were examined by using electrochemistry characterization. Tafel and CV curves from simulating electrolyte suggested that their corrosion potentials were in the following order: Ni﹥C﹥SS﹥Fe﹥Cu﹥Pb–Ag. As expected, the desulfurization ratio and cell voltage from bauxite electrolysis were in the following order respectively: Cu﹥Ni﹥Fe﹥SS﹥C﹥Pb–Ag and Ni﹥Fe﹥SS﹥Cu﹥C﹥Pb–Ag. Finally, Ni was proposed a kind of excellent electrode material for bauxite desulfurization from electrolysis.

关键词： Corrosion resistance High sulfur bauxite Electrolysis desulfurization Electrode materials

Bifunctional Catalyst of Cumn-Hzsm-5 for Selective Catalytic Reduction of No and Co Oxidation Under Oxygen Atmosphere

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SSRN 2022年

作者： Guo, Yangyang Zheng, Yang Peng, Yue Yue, Tao Zhu, Tingyu CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Innovation Academy for Green Manufacture Chinese Academy of Sciences Beijing100190 China School of Energy and Environmental Engineering University of Science and Technology Beijing Beijing100083 China Tsinghua University School of Environment State Key Joint Laboratory Environment Simulation and& Pollution Control Beijing100084 China Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen361021 China

Simultaneous removal of NOx and CO from steel sintering has attracted great attention because it is difficult to balance catalyst reducibility and surface acidity merely using metal oxides or zeolite catalysts. In this study, a mixed CuMn-HZSM-5 catalyst was prepared via an impregnation method. The optimized sample exhibited excellent performance with 90% NO conversion and 100% CO conversion at 175°C. The activity window of the catalyst was coincident with the actual demand of sintering flue gas control in 150-250°C. The active component CuMn suppressed the excessive Brønsted acid sites on the zeolite support for NH3 adsorption, while the reducibility of the catalyst also decreased compared with that of pure CuMn metal oxides. This synergistic effect was beneficial for the reduction of NH3 nonselective oxidation with O2. In addition, both the DFT and DRIFTS results revealed that NO conversion was improved by CO introduction at low temperature, since NO could adsorb on the CO-preadsorbed sites for the reduction to N2 via the O atoms of Mn3c sites, i.e., adsorbed CO could also serve as a reductant to reduce NO to N2, which provides another reaction pathway in SCR reactions. Moreover, the NO2- and N2O2- species were observed in the spectra as key intermediates to oxidize CO to CO2, which are also the promoters of CO control. © 2022, The Authors. All rights reserved.

关键词： Zeolites