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Hierarchically Porous Few-Layer Carbon Nitride and Its High H+Selectivity for Efficient Photocatalytic Seawater Splitting

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Nano Letters 2023年第10期23卷 4390-4398页

作者： Shi-Tian Xiao Rui Yin Lu Wu Si-Ming Wu Ge Tian Menny Shalom Li-Ying Wang Yi-Tian Wang Fu-Fei Pu Hannah-Noa Barad Fazhou Wang Xiao-Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering & State Key Laboratory of Silicate Materials for Architectures & Shenzhen Research Institute Wuhan University of Technology Wuhan 430070 China Key Laboratory for the Synthesis and Application of Organic Functional Molecules Ministry of Education College of Chemistry and Chemical Engineering Hubei University Wuhan 430062 China Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics National Center for Magnetic Resonance in Wuhan Wuhan Institute of Physics and Mathematics Innovation Academy for Precision Measurement Science and Technology Chinese Academy of Sciences Wuhan 430071 China Department of Chemistry Institute of Nanotechnology & Advanced Materials Bar Ilan University Ramat Gan 5290002 Israel

Photocatalysts for seawater splitting are severely restricted because of the presence of multiple types of ions in seawater that cause corrosion and deactivation. As a result, new materials that promote adsorption of H+and hinder competing adsorption of metal cations should enhance utilization of photogenerated electrons on the catalyst surface for efficient H2production. One strategy to design advanced photocatalysts involves introduction of hierarchical porous structures that enable fast mass transfer and creation of defect sites that promote selective hydrogen ion adsorption. Herein, we used a facile calcination method to fabricate the macro–mesoporous C3N4derivative, VN-HCN, that contains multiple nitrogen vacancies. We demonstrated that VN-HCN has enhanced corrosion resistance and elevated photocatalytic H2production performance in seawater. Experimental results and theoretical calculations reveal that enhanced mass and carrier transfer and selective adsorption of hydrogen ions are key features of VN-HCN that lead to its high seawater splitting activity.

关键词： Adsorption Defects in solids Ions Nitrogen Seawater

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External field-assisted catalysis

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eScience 2025年

作者： Linbo Jiang Lintao Jiang Xu Luo Ruidong Li Qingqu Zhou Weihao Zeng Jun Yu Lei Chen Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070 China

In recent years, substantial effort has been dedicated to improving the intrinsic catalytic activity of catalysts through structural modification, component regulation, and chemical state optimization. However, complexity in the design and construction of catalysts, and the possibility of encountering performance ceilings, may constrain their widespread use. Currently, the introduction of in situ external fields, such as force, electric, magnetic, acoustic, light, and thermal fields, is an attractive approach to enhance the catalytic efficiency of catalysts. Such in situ physical fields feature continuity, reversibility, and controllability, and can exert external force or energy on catalysts, thereby affecting their microscopic structures and electron arrangements, accelerating their mass transfer and reaction kinetics. Mutual coupling and conversion among different external fields are also worth exploring. Various in situ external field effects work in multifaceted ways to promote catalysis in energy-environment systems by optimizing mass/energy transfer processes, modifying structures, and accelerating catalytic reaction kinetics, thereby significantly improving the catalytic properties of materials. This review summarizes and analyzes the latest developments in external field-assisted methods for boosting catalyst performance. The external field effect, related catalysis mechanism, and external field-enhanced catalysis are highlighted, and we discuss future challenges, countermeasures, and opportunities for external field-assisted catalysis and beyond.

关键词： Catalysis External field Field-assisted effects Reaction mechanism

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Energetic Mof-Derived Hollow Carbon Tubes with Interconnected Channels and Encapsulated Nickel-Cobalt Alloy Sites as Bifunctional Catalysts for Zn–Air Batteries with Stable Cycling Over 600 Cycles

SSRN

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SSRN 2022年

作者： Duan, Xin-De Zhu, Jia-Wei Zheng, He-Gen State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Collaborative Innovation Center of Advanced Microstructures Nanjing University Jiangsu Nanjing210023 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China

Energetic metal–organic frameworks (EMOFs) and EMOF-derived materials are currently a hot spot to replace precious-metal electrocatalysts. Here, the reasonable strategy and synthesis of an inventive class of alloy@C materials from EMOFs via one-step pyrolysis is reported as the first example. The freshly progressive NiCo@C with a individual hierarchical structure, being composed of uniformly distributive metal alloy nanoparticles (MANPs) decorated by N-doped porous hollow carbon nanotubes (HCNTs), displays extraordinary bifunctional catalytic activities for oxygen reduction and oxygen evolution reactions (ORR and OER) than that of commercial precious-metal catalysts. Experimental characterizations and theoretical calculations reveal the vital role of Ni-Co alloy doping in adjusting both performances. Moreover, as an air electrode in Zn–air batteries, NiCo@C demonstrates a large peak power density of 170 mW cm−2 and superior long-term stability over 600 cycles. In consideration of the expansive category of EMOFs and the governable fixation of single/multiple metal particles, this strategy gives evidence of a capacious scientific range. © 2022, The Authors. All rights reserved.

关键词： Nickel alloys

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Improvement of Sic Deposition Uniformity in Cvd Reactor by Showerhead with Baffle

SSRN

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SSRN 2023年

作者： Li, Qizhong Zhang, Yixuan Ji, Baifeng Zhang, Song Tu, Rong Hubei Key Laboratory of Advanced Technology for Automotive Components Wuhan University of Technology Wuhan430070 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China School of Civil Engineering and Architecture Wuhan University of Technology Wuhan430070 China Chaozhou Branch of Chemistry and Chemical Engineering Guangdong Laboratory Chaozhou521000 China Wuhan University of Technology Advanced Engineering Technology Research Institute of Zhongshan City Guangdong Zhongshan528400 China

The deposition rate distribution during halide chemical vapour deposition of silicon carbide (SiC) is influenced by equipment structure, and a uniform film can be obtained by optimising the chamber structure. A detailed chemical reaction mechanism was incorporated into a reaction chamber model to verify the SiC deposition kinetics model. We studied the influence of spray hole size, baffle size, and baffle positioning on the deposition rate uniformity. The results show that reducing the size of the spray holes leads to a "double peak" in the deposition rate across the substrate from the edge to both sides, which first increases and then decreases. The "double peak" disappears when the spray hole size is reduced. With an increase in baffle size, the uniformity of the deposition rate first increased and then decreased. Moreover, the baffle displacement had little effect on the deposition rate when the baffle-to-spray plate distance was at least 45 mm. Meanwhile, the deposition uniformity gradually worsened when the baffle distance was reduced. The spray plate and baffle reduced the extreme difference in deposition rates across the effective deposition area by improving the velocity field of the reaction chamber. A uniform SiC film can be obtained using the proposed optimisation method. © 2023, The Authors. All rights reserved.

关键词： Structural optimization

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Cell-interface engineering of Shewanella oneidensis MR-1 for enhanced stability of viability and functions

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Colloids and Surfaces B: Biointerfaces 2025年 254卷 114862页

作者： Zhang, Tong-Kai Liu, Jie Yi, Zi-Qian Ye, Kai-Qi Geng, Wei Huang, Yao-Qi Tian, Ge Yang, Xiao-Yu State Key Laboratory of Silicate Materials for Architectures & State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Chemistry Chemical Engineering and Life Sciences & Laoshan Laboratory & School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China School of Engineering and Applied Sciences Harvard University Cambridge 02138 MA United States National energy key laboratory for new hydrogen-ammonia energy technologies Foshan Xianhu Laboratory Foshan 528200 China

Creating synthetic interface from non-life materials to improve Shewanella stability and endow them with precise functionalities could revolutionize cell-based biotechnologies. Herein, a stable and cytoprotective biointerface on Shewanella surface are rapidly generated through immediate coordination complexes of TA and Fe (Ⅲ) ions. TA-Fe^Ⅲ-based biointerface engineered Shewanella cells can be endowed with extremophile properties of resistance to high temperature, osmotic stress, UV light and lysozyme, and can be released from TA-Fe^Ⅲ biointerface through the acidic condition-triggered decomplexation. Furthermore, various functional materials with abiotic properties like conductivity and magnetism can be induced onto surface of Shewanella through co-self-assembly with TA-Fe^Ⅲ interface. © 2025 Elsevier B.V.

关键词： Cell-interface engineering Cytoprotective Degradable Precise functions TA-FeⅢ

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Al-Doped Nb2o5/Carbon Micro-Particles Anodes for High Rate Lithium-Ion Batteries

SSRN

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SSRN 2022年

作者： Zhu, Zhu Liu, Fang Wang, Hong Yu, Ruohan Wu, Jinsong State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Hubei Wuhan430070 China Wuhan University of Technology Wuhan430070 China

Orthorhombic niobium pentoxide (T-Nb2O5 ) has attracted extensive attention in the field of ultra-fast lithium ion batteries (LIBs) due to its high rate performance. However, its instability at a low potential and inherent low conductivity limits its fast charging capability. Here, microspheres of aluminum-doped T-Nb2O5 embedded in N-doped carbon network (Al-Nb2O5@NC) are prepared. The effects of Al-doping on the crystal structure and electrochemical properties are systematically studied. It is found that Al-doping has led to increase of the density of O2- vacancies and then low-oxidized state Nb4+ ions, improving ionic and electrical conductivity. The substitution of Al3+ ions for Nb5+ ions improves the lattice stability, reduces the undesirable migration of Nb in cycling, and stabilizes the capacity during fast charging. The LIBs using Al-Nb2O5@NC as anode have high rate performance and cycling stability ( i.e. , ~82 mAh g-1 at 20 A g-1 after 9900 cycles). Meanwhile, the intercalation-type electrochemical reaction is verified by in-situ transmission electron microscope (TEM), by which it is found that Al-Nb2O5@NC has better crystalline integrity. By integrating Al doping and carbon network, the micron-size Al-Nb2O5@NC particles developed in this work are promising anodes to build fast charge/discharge LIBs with high specific capacity, stability and excellent rate performance. © 2022, The Authors. All rights reserved.

关键词： Lithium-ion batteries

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Effect of pH, milling time, and Isobam content on porous silicon nitride ceramics prepared by gel casting

Advanced Powder Materials

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advanced Powder Materials 2023年第1期2卷 100-107页

作者： Hailing Yang Zhi Wang Mengyong Sun Fei Chen Jun Ji Sique Chen Yingying Chen Deli Ma Zhenyu Zhang Baocai Pan Yulin Wei Qinggang Li Shandong Provincial Key Laboratory of Preparation and Measurement of Building Materials University of JinanJinan 250022China School of Material Science and Engineering University of JinanJinan 250022China No.52 Institute of China North Industry Group Yantai 264003China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

As a non-toxic copolymer of isobutylene and maleic anhydride,Isobam is successfully used as a dispersant and a gelling agent for fabricating porous Si_(3)N_(4) ceramics by gel *** dispersity and rheological properties of the Si_(3)N_(4) slurry are influenced by the pH,milling time,and Isobam content which varies from 0.1 wt.%to 0.6 wt.%,and these factors are *** slurry with 40 vol.%solid content and milled for 4 h has a high zeta potential at pH 12(adjusted by Tetramethyl ammonium hydroxide(TMAH)),which means that the particles are well *** mechanisms of TMAH are electrostatic repulsion and steric *** viscosity of the slurry increases with the increase of Isobam *** pressureless sintering at 1700℃ for 2 h,a uniform unique interlocking microstructure of rod-like β-Si_(3)N_(4) grains is observed,which may improve the flexural strength of the ceramics by intergranular fracture and particle pullout of β-Si_(3)N_(4) *** density and porosity of the samples fluctuate negligibly with the increase of Isobam content,and the Si_(3)N_(4) ceramic with 0.1 wt.% Isobam exhibits the highest bending strength of 251.6 MPa among all samples.

关键词： Si_(3)N_(4)ceramics Viscosity Zeta potential Gel casting Isobam

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Recent progress in perovskite solar cells:from device to commercialization

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Science China Chemistry 2022年第12期65卷 2369-2416页

作者： Xinhui Luo Xuesong Lin Feng Gao Yang Zhao Xiaodong Li Liqing Zhan Zexiong Qiu Jin Wang Cong Chen Lei Meng Xiaofeng Gao Yu Zhang Zijian Huang Rundong Fan Huifen Liu Yanrun Chen Xiaoxue Ren Jiahong Tang Chun-Hao Chen Dong Yang Yongguang Tu Xiao Liu Dongxue Liu Qing Zhao Jingbi You Junfeng Fang Yongzhen Wu Hongwei Han Xiaodan Zhang Dewei Zhao Fuzhi Huang Huanping Zhou Yongbo Yuan Qi Chen Zhaokui Wang Shengzhong(Frank)Liu Rui Zhu Jotaro Nakazaki Yongfang Li Liyuan Han State Key Laboratory of Metal Matrix Composites School of Material Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Lab for Mesoscopic Physics and Frontiers Science Center for Nano-optoelectronics School of PhysicsPeking UniversityBeijing 100871China Key Laboratory of Semiconductor Materials Science Institute of SemiconductorsChinese Academy of SciencesBeijing 100083China School of Physics and Electronic Science Engineering Research Center of Nanophotonics&Advanced InstrumentMinistry of EducationEast China Normal UniversityShanghai 200241China Key Laboratory for Advanced Materials and Institute of Fine Chemicals School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China Institute of Photoelectronic Thin Film Devices and Technology Renewable Energy Conversion and Storage CenterSolar Energy Research CenterNankai UniversityTianjin 300350China College of Materials Science and Engineering&Engineering Research Center of Alternative Energy Materials&Devices Ministry of EducationSichuan UniversityChengdu 610065China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationSchool of Materials Science and EngineeringPeking UniversityBeijing 100871China School of Physics and Electronics Hunan Key Laboratory of Nanophotonics and DevicesCentral South UniversityChangsha 410083China Experimental Center for Advanced Materials School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Jia

Perovskite solar cells(PSCs) are undergoing rapid development and the power conversion efficiency reaches 25.7% which attracts increasing attention on their commercialization *** this review,we summarized the recent progress of PSCs based on device structures,perovskite-based tandem cells,large-area modules,stability,applications and ***,the challenges and perspectives are discussed,aiming at providing a thrust for the commercialization of PSCs in the near future.

关键词： perovskite solar cells device engineering stability application

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Stable Cycling of High-Capacity Red Phosphorus/Carbon Composite Anode in All-Solid-state Lithium-Ion Batteries

SSRN

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SSRN 2023年

作者： Sun, Han Liu, Dan Li, Jing Qu, Deyu Xie, Zhizhong Song, Jiangping Tang, Haolin Department of Chemistry School of Chemistry Chemical Engineering and Life Sciences Wuhan University of Technology 122 Luoshi Road Wuhan430070 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan430070 China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan528200 China

Using the Li metal anode in all-solid-state batteries (ASSBs) is challenging than initially envisioned owing to poor thermodynamic stability against solid electrolytes. Therefore, it is imperative to develop Li-ion anode alternatives for the future practical implementation of high-energy ASSBs. Here, for the first time, we demonstrate the stable cycling of red phosphorus (P)-carbon composite as a low-cost and high-capacity anode in sulfide electrolyte-based ASSBs. By loading subnanometer-scaled red P clusters in the micropores of a commercial activated carbon (AC), the electrically insulating red P can be fully activated and operable in room-temperature ASSBs. Benefiting from its medium lithiation potential and fast Li+ diffusion capability, the resultant P@AC electrode enables a record-high current density of over 18 mA cm−2 without Li dendrite formation in a symmetric cell. In a half cell, the P@AC material with a red P content of 53 wt% can deliver a high first delithiation capacity of 1438 mAh g−1 at 0.2 A g−1 and a decent capacity retention of 66.9% after 400 cycles (running time of over 180 days). When paired with a LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, the P@AC||NCM811 full cell achieves an initial areal capacity of 2.98 mAh cm−2 and enables stable cycling over 200 cycles. © 2023, The Authors. All rights reserved.

关键词： Activated carbon

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Solid-state Stepwise Temperature-Programmable synthesis of Bioinspired Fe-N-C Oxygen Reduction Electrocatalyst Featuring Fe-N5 Configuration

SSRN

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SSRN 2024年

作者： Sang, Wei Chaemchuen, Somboon Zhang, Longyang Wang, Zechen Li, Xingchuan Nagasaka, Cocoro Andrew Xiong, Mo Ogiwara, Naoki Chen, Cheng Verpoort, Francis Mu, Shichun Kou, Zongkui State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan430070 China Department of Basic Science School of Arts and Sciences The University of Tokyo Komaba Meguro-ku Tokyo153-8902 Japan MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter School of Physics Xi’an Jiao tong University Xi’an710049 China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya572000 China

The bioinspired Fe-N-C features an asymmetric Fe-N5 configuration to produce active metal-oxygen intermediates by introducing axial N ligand into a symmetric Fe-N4 structure, enabling highly active oxygen reduction reaction (ORR). However, the artificial creation of active Fe-N5 configuration with a direct, facile and green method is still pendent, as current techniques involve complex processes and costly precursors. Herein, we develop a novel solid-state stepwise temperature-programmable (SST) route to directly produce bioinspired Fe-N5-C. We then demonstrate that Fe-N5-C exhibit a quite higher half-wave potential (0.92 V) with 22-fold faster ORR kinetics (15.6 mA cm−2 @ 0.85 V) than that of the commercial Pt/C counterpart. Indeed, we perform density functional theory (DFT) to find that the Fe is charged with an extra 0.1 e− through the axially coordinate N ligand, which significantly enhances the ability to activate O2 and enables an easier desorption of the crucial intermediate *OH on the Fe-N5 configuration over the conventional Fe-N4 structure. © 2024, The Authors. All rights reserved.

关键词： Density functional theory

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