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Interfacial coordination bonds accelerate charge separation for unprecedented hydrogen evolution over S-scheme heterojunction

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Chinese Journal of Catalysis 2024年第10期65卷 174-184页

作者： Chunxue Li Hao Lu Guixiang Ding Tianyi Ma Shiyong Liu Li Zhang Guangfu Liao College of Ecological Environment and Urban Construction Fujian University of TechnologyFuzhou 350118FujianChina School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou 215009JiangsuChina College of Materials Engineering Fujian Agriculture and Forestry UniversityFuzhou 350002FujianChina School of Science RMIT UniversityMelbourneVIC 3000Australia Jiangxi Province Key Laboratory of Functional Crystalline Materials Chemistry Jiangxi University of Science and TechnologyGanzhou 341000JiangxiChina State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile UniversityWuhan 430200HubeiChina

Inspired by natural photosynthesis,fabricating high-performance S-scheme heterojunction is regarded as a successful tactic to address energy and environmental ***,NH_(2)-MIL-125(Ti)/Zn_(0.5)Cd_(0.5)S/NiS(NMT/ZCS/NiS)S-scheme heterojunction with interfacial coordination bonds is successfully synthesized through in-situ solvothermal ***,the optimal NMT/ZCS/NiS S-scheme heterojunction exhibits comparable photocatalytic H_(2)evolution(PHE)rate of about 14876.7μmol h^(−1)g^(−1)with apparent quantum yield of 24.2%at 420 nm,which is significantly higher than that of recently reported MOFs-based *** interfacial coordination bonds(Zn–N,Cd–N,and Ni–N bonds)accelerate the separation and transfer of photogenerated charges,and the NiS as cocatalyst can provide more catalytically active sites,which synergistically improve the photocatalytic ***,theoretical calculation results display that the construction of NMT/ZCS/NiS S-scheme heterojunction also optimize the binding energy of active site-adsorbed hydrogen atoms to enable fast adsorption and *** Kelvin probe force microscopy,in-situ irradiation X-ray photoelectron spectroscopy,femtosecond transient absorption spectroscopy,and theoretical calculations provide sufficient evidence of the S-scheme charge migration *** work offers unique viewpoints for simultaneously accelerating the charge dynamics and optimizing the binding strength between the active sites and hydrogen adsorbates over S-scheme heterojunction.

关键词： Interfacial coordination bond S-schemeheterojunction Photocatalytic H_(2)evolution Charge dynamics Free energy barrier

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Cathodic Zn underpotential deposition:an evitable degradation mechanism in aqueous zinc-ion batteries

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Science Bulletin 2022年第18期67卷 1882-1889,M0004页

作者： Shaohua Zhu Yuhang Dai Jinghao Li Chumei Ye Wanhai Zhou Ruohan Yu Xiaobin Liao Jiantao Li Wei Zhang Wei Zong Ruwei Chen Guanjie He Dongliang Chao Qinyou An State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materialsand School of Chemistry and MaterialsFudan UniversityShanghai 200433China Christopher Ingold Laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Electrochemical Innovation Laboratory Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUK State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China Department of Materials Science and Metallurgy University of CambridgeCambridge CB30FSUK

Aqueous zinc-ion batteries(AZIBs)are promising for large-scale energy storage,but their development is plagued by inadequate cycle ***,for the first time,we reveal an unusual phenomenon of cathodic underpotential deposition(UPD)of Zn,which is highly irreversible and considered the origin of the inferior cycling stability of *** experimental and theoretical simulation approaches,we propose that the UPD process agrees with a two-dimensional nucleation and growth model,following a thermodynamically feasible ***,the universality of Zn UPD is identified in systems,including VO_(2)//Zn,TiO_(2)//Zn,and SnO_(2)//*** practice,we propose and successfully implement removing cathodic Zn UPD and substantially mitigate the degradation of the battery by controlling the end-ofdischarge *** work provides new insights into AZIBs degradation and brings the cathodic UPD behavior of rechargeable batteries into the limelight.

关键词： Underpotential deposition Zn metal deposition Zinc-ion battery Aqueous battery Degradation mechanism

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Interaction of the Initial β-Mg17Al12 Phase with α-Matrix Grains in the AZ91 Magnesium Alloy During Hot Extrusion

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SSRN 2025年

作者： Zhao, Dijia Shao, Yuman Lü, Shulin Yan, Zhaoxiang Guo, Wenbo Li, Shilong Li, Jianyu Xu, Shiwei Wu, Shusen Nie, Jianfeng State Key Laboratory of Materials Processing and Die & Mould Technology Huazhong University of Science and Technology Wuhan430074 China State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body Hunan University Changsha410082 China Department of Materials Science and Engineering Monash University VIC3800 Australia

Secondary phase particles in magnesium alloys can facilitate particle-stimulated nucleation and pinning the grain boundary migration during the dynamic recrystallization (DRX) process. But a conflict exists between these two effects. By optimizing the hot extrusion process and preserving the irregular island-shaped β-Mg17Al12 phase (β-phase) derived from the eutectic reaction in the AZ91 magnesium alloy billet, we revealed the interaction of the initial β-phase with the α-matrix during extrusion. In the early stages of extrusion, the irregular, island-shaped, coarse β-phase causes significant dislocation accumulation in the adjacent α-matrix due to the hardness difference. As dislocations accumulate, the β-phase fragments and transforms into spindly fibrous bands, effectively illustrating a pinning effect. The morphological change of the β-phase not only promotes the DRX process but also inhibits the growth of DRXed grains, thereby refining the grain size. This research helps to expand the design strategies for extruded magnesium alloys. © 2025, The Authors. All rights reserved.

关键词： Magnesium alloys

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Tellurium Filled Carbon Nanotubes Cathodes for Li-Te Batteries with High Capacity and Long-Term Cyclability

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SSRN 2023年

作者： Rao, Shaoqing Wu, Ruizhe Zhu, Zhu Wu, Jinsong Ding, Yao Mai, Liqiang School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules College of Chemistry and Chemical Engineering Hubei University Wuhan430062 China

Li-Te batteries, compared with traditional lithium-ion batteries and Li-other group VIA elements (including O, S, Se) batteries, have shown overwhelming features of high specific volumetric capacity and superior electrical conductivity. These features make the Li-Te batteries possess great importance in modern portable electronics and electric vehicles with limited battery package size. However, the Achilles' Heel in Li-Te batteries is the huge volume change and inevitable shuttle effect of polytellurides during cycling. Herein, we synthesize a cathode material based on polycrystalline Te encapsulated in N-doped multiwall carbon nanotubes (Te-filled CNTs) by physical vapor transport (PVT) method. With unique spatial restriction of the CNT hosts, the electrochemically active Te content can be well preserved, and the prepared Te-filled CNTs cathodes deliver a high specific capacity of 590 mAh g-1 based on Te content. More importantly, the reaction kinetics and electrochemical reversibility of the cathodes have been significantly improved by using nanoscale cavities (4-6 nm) by which the polytellurides are stabilized. Meanwhile, a series of in situ Raman, XRD and TEM characterizations are carried out to reveal a two-step discharge/charge mechanism for Te-filled CNTs, which is the key for the excellent cycling stability. In addition, theoretical calculations prove that the encapsulated Te ensure a lower energy barrier for lithiation compared with bare CNT. This work sheds light on the nanoconfinement effect of CNT for improving the utilization and cycling stability of Te in Li-Te batteries, and provides a new strategy of designing high-performance group VIA element based cathodes. © 2023, The Authors. All rights reserved.

关键词： Cathodes

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Microstructural Evolution of Defects Under Proton Irradiation in Porous Cu

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SSRN 2023年

作者： Li, Honglin Wang, Hao Wen, Pin Huang, Zhifeng Yin, Guanchao Chen, Fei Hubei Longzhong Laboratory Xiangyang441106 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics School of Science Wuhan University of Technology Wuhan430070 China Wuhan University of Technology China

The high specific strength and exceptional thermal insulating properties of porous metals make them an ideal choice for aerospace structural components and thermal insulation materials. However, in the space environment, proton irradiation leads to the formation of voids, bubbles, and dislocation loops, significantly compromising their physical and mechanical properties. To date, there has been limited attention to the radiation resistance properties in research related to porous metals. This study conducted proton irradiation experiments with a total dose of 1×1017 ions/cm2 on porous Cu. This study discusses and explains the irradiation-induced damage characteristics on the surface of porous Cu before and after proton irradiation. This provides insights into the radiation damage mechanisms within the porous Cu ligaments and the hydrogen release behavior on the ligament surface. Cascade recoil and collision-induced thermal spike effects modify material defect characteristics and crystal structure. This study elucidates the defect evolution mechanism of porous materials under proton irradiation, offering new insights for the design of other radiation-resistant porous materials as protective materials for future advanced space probes. © 2023, The Authors. All rights reserved.

关键词： Radiation damage

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Crystalline porous materials:from zeolites to metal-organic frameworks(MOFs)

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Frontiers of Chemical Science and Engineering 2020年第2期14卷 123-126页

作者： Zaiku Xie Bao-Lian Su State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Sinopec Shanghai Research Institute of Petrochemical TechnologyShanghai 201208China Laboratory of Inorganic Materials Chemistry(CMI) University of NamurNamurBelgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430074China

As a class of important crystalline porous materials,zeolites which were first found in 1756 have now been widely used in chemical industries for catalysis,adsorption and separation.35232 patents with the title including Hzeolite*n are documented by Derwent Innovations Index on January 2,2020[1].Despite of spread applications of zeolites and related-materials in industry,fundamental research of zeolites and their applications are still desired in both academia and industry,as shown in Fig.1.

关键词： porous zeolites zeolite

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Tuning the strength of built-in electric field in 2D/2D g-C_(3)N_(4)/MS_(2) and g-C_(3)N_(4)/ZrS_(2) S-scheme heterojunctions by nonmetal doping

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Journal of Materiomics 2021年第5期7卷 988-997页

作者： Bicheng Zhu Haiyan Tan Jiajie Fan Bei Cheng Jiaguo Yu Wingkei Ho State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology122 Luoshi RoadWuhan430070China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou450001China Department of Science and Environmental Studies The Education University of Hong KongTai PoN.T.Hong Kong999077China

Single photocatalysts usually exhibit unsatisfactory performance due to the serious recombination of photogenerated electron‒hole *** two photocatalysts to construct S-scheme heterojunction could solve this *** S-scheme mechanism,the interfacial built-in electric field(IEF)provides a vital driving force for efficient charge *** the IEF is a feasible strategy to further improve the photocatalytic ***,a novel idea of tuning the strength of IEF in 2D/2D graphitic carbon nitride(g-C_(3)N_(4))/MS2(M=Sn,Zr)S-scheme heterojunctions by nonmetal doping was developed by employing density functional theory *** nonmetal elements(O,P,and S)were severally introduced into g-C_(3)N_(4)/MS_(2) *** density difference suggested that O and S doping led to increased interfacial electron transfer,while P doping had minimal *** expected,the calculated field strength of O-and S-doped g-C_(3)N_(4)/MS_(2) composites was significantly larger than that of pristine and P-doped g-C_(3)N_(4)/MS_(2) ***,O and S doping endowed g-C_(3)N_(4)/MS_(2) Sscheme heterojunctions with enhanced IEF and more thorough charge ***,the experimentally synthesized O-C_(3)N_(4)/ZrS_(2) composite exhibited better photocatalytic H2-production activity than g-C_(3)N_(4)/ZrS_(2) *** work proposed an original idea of employing proper nonmetal doping to magnify the advantage of S-scheme heterojunction in accelerating charge separation.

关键词： Graphitic carbon nitride Density functional theory Field strength Photocatalysis Van der Waals heterostructure

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Application of novel nanobubble-contained electrolyzed catalytic water to cleanup petroleum-hydrocarbon contaminated soils and groundwater: A pilot-scale and performance evaluation study

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Journal of Environmental Management 2023年 347卷 119058页

作者： Ho, Wing-Sze Lin, Wei-Han Verpoort, Francis Hong, Kun-Liang Ou, Jiun-Hau Kao, Chih-Ming Institute of Environmental Engineering National Sun Yat-Sen University Kaohsiung Taiwan State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan China Suzhou Dingdedian Environmental Protection Technology Co. Ltd. Suzhou China

Soil and groundwater contamination caused by petroleum hydrocarbons is a severe environmental problem. In this study, a novel electrolyzed catalytic system (ECS) was developed to produce nanobubble-contained electrolyzed catalytic (NEC) water for the remediation of petroleum-hydrocarbon-contaminated soils and groundwater. The developed ECS applied high voltage (220 V) with direct current, and titanium electrodes coated with iridium dioxide were used in the system. The developed ECS prototype contained 21 electrode pairs (with a current density of 20 mA/cm2), which were connected in series to significantly enhance the hydroxyl radical production rate. Iron-copper hybrid oxide catalysts were laid between each electrode pair to improve the radical generation efficiency. The electron paramagnetic resonance (EPR) and Rhodamine B (RhB) methods were applied for the generated radical species and concentration determination. During the operation of the ECS, high concentrations of nanobubbles (nanobubble density = 3.7 × 109 particles/mL) were produced due to the occurrence of the cavitation mechanism. Because of the negative zeta potential and nano-scale characteristics of nanobubbles (mean diameter = 28 nm), the repelling force would prevent the occurrence of bubble aggregations and extend their lifetime in NEC water. The radicals produced after the bursting of the nanobubbles would be beneficial for the increase of the radical concentration and subsequent petroleum hydrocarbon oxidation. The highly oxidized NEC water (oxidation-reduction potential = 887 mV) could be produced with a radical concentration of 9.5 × 10−9 M. In the pilot-scale study, the prototype system was applied to clean up petroleum-hydrocarbon polluted soils at a diesel-oil spill site via an on-site slurry-phase soil washing process. The total petroleum hydrocarbon (TPH)-contaminated soils were excavated and treated with the NEC water in a slurry-phase reactor. Results show that up to 74.4% of TPH (initial

关键词： Soils

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Biomedical polymers: synthesis, properties, and applications

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Science China Chemistry 2022年第6期65卷 1010-1075页

作者： Wei-Hai Chen Qi-Wen Chen Qian Chen Chunyan Cui Shun Duan Yongyuan Kang Yang Liu Yun Liu Wali Muhammad Shiqun Shao Chengqiang Tang Jinqiang Wang Lei Wang Meng-Hua Xiong Lichen Yin Kuo Zhang Zhanzhan Zhang Xu Zhen Jun Feng Changyou Gao Zhen Gu Chaoliang He Jian Ji Xiqun Jiang Wenguang Liu Zhuang Liu Huisheng Peng Youqing Shen Linqi Shi Xuemei Sun Hao Wang Jun Wang Haihua Xiao Fu-Jian Xu Zhiyuan Zhong Xian-Zheng Zhang Xuesi Chen Key Laboratory of Biomedical Polymers of Ministry of Education&Department of Chemistry Wuhan UniversityWuhan430072China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin300350China Key Laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of Chemical Technology) Ministry of EducationBeijing Laboratory of Biomedical MaterialsCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing100029China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou310027China State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials of Ministry of EducationCollege of ChemistryNankai UniversityTianjin300071China Key Laboratory of Advanced Drug Delivery Systems of Zhejiang Province College of Pharmaceutical SciencesZhejiang UniversityHangzhou310058China Jinhua Institute of Zhejiang University Jinhua321299China Zhejiang Key Laboratory of Smart BioMaterials and Center for Bionanoengineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China ZJU-Hangzhou Global Scientific and Technological Innovation Center Hangzhou311215China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science and Laboratory of Advanced MaterialsFudan UniversityShanghai200438China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in Nano-scienceNational Center for Nanoscience and Technology(NCNST)Beijing100190China School of Biomedical Sciences and Engineering Guangzhou International CampusSouth China University of TechnologyGuangzhou510006China Institute of Functional Nano and So

Biomedical polymers have been extensively developed for promising applications in a lot of biomedical fields, such as therapeutic medicine delivery, disease detection and diagnosis, biosensing, regenerative medicine, and disease treatment. In this review, we summarize the most recent advances in the synthesis and application of biomedical polymers, and discuss the comprehensive understanding of their property-function relationship for corresponding biomedical applications. In particular, a few burgeoning bioactive polymers, such as peptide/biomembrane/microorganism/cell-based biomedical polymers, are also introduced and highlighted as the emerging biomaterials for cancer precision therapy. Furthermore, the foreseeable challenges and outlook of the development of more efficient, healthier and safer biomedical polymers are discussed. We wish this systemic and comprehensive review on highlighting frontier progress of biomedical polymers could inspire and promote new breakthrough in fundamental research and clinical translation.

关键词： biomedical polymer nanomedicine cancer therapy drug delivery bioimaging and biosensing tissue engineering regenerative medicine cytotoxicity biocompatibility

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Operando-reconstructed polyatomic ion layers boost the activity and stability of industrial current–density water splitting

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Science Bulletin 2024年第21期69卷 3384-3394页

作者： Yingxia Zhao Ying Wu Qunlei Wen Danji Huang Ruoou Yang Haozhi Wang Yingying Xu Ming Sun Youwen Liu Jiakun Fang Tianyou Zhai Lin Yu Guangdong Engineering Technology Research Center of Modern Fine Chemical Engineering School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006China State Key Laboratory of Materials Processing and Die&Mould Technology and School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Advanced Electromagnetic Engineering and Technology and School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510641China Analysis and Test Center Guangdong University of Technology Guangdong University of TechnologyGuangzhou 510006China State Key Laboratory of Marine Resource Utilization in South China Se1 School of Materials Science and EngineeringHainan UniversityHaikou 570228China

Metal–organic frameworks have garnered attention as highly efﬁcient pre-electrocatalysts for the oxygen evolution reaction(OER).Current structure–activity relationships primarily rely on the assumption that the complete dissolution of organic ligands occurs during ***,modeling based on NiFe Prussian blue analogs(NiFe-PBAs)show that cyanide ligands leach from the matrix and subsequently oxidize to corresponding inorganic ions(ammonium and carbonate)that re-adsorb onto the surface of NiFe OOH during the OER ***,the surface-adsorbed inorganic ions induce the OER reaction of NiFe OOH to switch from the adsorbate evolution to the lattice-oxygen–mediated mechanism,thus contributing to the high *** addition,this reconstructed inorganic ion layer acting as a versatile protective layer can prevent the dissolution of metal sites to maintain contact between catalytic sites and reactive ions,thus breaking the activity–stability ***,our constructed NiFePBAs exhibit excellent durability for 1250 h with an ultralow overpotential of 253 mV at 100 mA cm*** scale-up NiFe-PBAs operated with a low energy consumption of4.18 kWh m3 H2 in industrial water electrolysis *** economic analysis of the entire life cycle demonstrates that this green hydrogen production is priced at US$2.59 kg^(-1)H_(2),meeting global targets(

关键词： Chemical recognition Oxygen evolution mechanism Industrial water electrolysis

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