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Light-assisted preparation of heterostructured g-C 3 N 4 /ZnO nanorods arrays for enhanced photocatalytic hydrogen performance

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Catalysis Today 2020年 355卷 932-936页

作者： Jing Liu Xiao-Ting Yan Xu-Sen Qin Si-Jia Wu Heng Zhao Wen-Bei Yu Li-Hua Chen Yu Li Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Nanostructure Research Centre (NRC) Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Clare Hall University of Cambridge Herschel Road Cambridge CB3 9AL United Kingdom

The type II heterostructured g-C 3 N 4 /ZnO nanorods arrays (NRAs) with intimate interface connection were successfully synthesized via a light-assisted method for photocatalytic H 2 production. Such type-II heterojunction between g-C 3 N 4 and ZnO not only promotes the charge separation and transport but also extends light absorption to the visible light region. In addition, the high physicochemical stability of g-C 3 N 4 layer keeps ZnO from photocorrosion during the reaction. Consequently, the heterostructured g-C 3 N 4 /ZnO NRAs demonstrate enhanced photocatalytic H 2 performance. In particular, the highest photocatalytic activity enhancement of g-C 3 N 4 /ZnO heterostructure is 3.3 times that of ZnO NRAs with a good stability of 85% retention rate after 5 cycles. Our work here presents an effective strategy to construct heterojunction between g-C 3 N 4 and metal oxide semiconductors for significantly enhanced photocatalytic H 2 production.

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Graphene oxide-decorated Fe2（MoO4）3 microflowers as a promising anode for lithium and sodium storage

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Nano Research 2018年第3期11卷 1285-1293页

作者： Chunhua Han Xiaoji Ren Qidong Li Wen Luo Lei Huang Liang Zhou Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Luoshi Road122 Wuhan 430070 China Laboratoire de Chimie et Physique: Approche Multiechelles des Milieux Complexes Institut Jean Barriol Universite de Lorraine57070 Metz France

Mixed transition metal oxides （MTMOs） have received intensive attention as promising anode materials for lithium-ion batteries （LIBs） and sodium-ion batteries （SIBs）. In this work, we demonstrate a facile one-step water-bath method for the preparation of graphene oxide （GO） decorated Fe2（MoO4）3 （FMO） microflower composite （FMO/GO）, in which the FMO is constructed by numerous nanosheets. The resulting FMO/GO exhibits excellent electrochemical performances in both LIBs and SIBs. As the anode material for LIBs, the FMO/GO delivers a high capacity of 1,220 mAh·g^-1 at 200 mA·g^-1 after 50 cycles and a capacity of 685 mAh·g^-1 at a high current density of 10 A·g^-1. As the anode material for SIBs, the FMO/GO shows an initial discharge capacity of 571 mAh·g^-1 at 100 mA·g^-1, maintaining a discharge capacity of 307 mAh·g^-1 after 100 cycles. The promising performance is attributed to the good electrical transport from the intimate contact between FMO and graphene oxide. This work indicates that the FMO/GO composite is a promising anode for high-performance lithium and sodium storage.

关键词： Fe2（MoO4）3 microflowers anode lithium and sodium storage

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Proton/Mg2+Co-Insertion Chemistry in Aqueous Mg-Ion Batteries: From the Interface to the Inner

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Angewandte Chemie 2023年第37期135卷

作者： Meng Huang Xuanpeng Wang Junjun Wang Jiashen Meng Xiong Liu Qiu He Lishan Geng Qinyou An Jinlong Yang Liqiang Mai Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen 518060 China Hainan Institute Wuhan University of Technology Sanya 572000 P. R. China Department of Physical Science & Technology School of Science Wuhan University of Technology Hubei Wuhan 430072 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China School of Materials Science and Engineering Zhengzhou University Zhengzhou 450001 China College of Materials Science and Engineering Sichuan University Chengdu 610065 China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 P. R. China

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Verifying the Charge-Transfer Mechanism in S-Scheme Heterojunctions Using Femtosecond Transient Absorption Spectroscopy

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Angewandte Chemie 2022年第8期135卷

作者： Chang Cheng Dr. Jianjun Zhang Dr. Bicheng Zhu Prof. Guijie Liang Prof. Liuyang Zhang Prof. Jiaguo Yu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 430070 Wuhan P. R. China Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street 430078 Wuhan P. R. China Hubei Key Laboratory of Low Dimensional Arts and Science Hubei University of Arts and Science 441053 Xiangyang P. R. China

The S-scheme heterojunction is flourishing in photocatalysis because it concurrently realizes separated charge carriers and sufficient redox ability. Steady-state charge transfer has been confirmed by other methods. However, an essential part, the transfer dynamics in S-scheme heterojunctions, is still missing. To compensate, a series of cadmium sulfide/pyrene- alt -difluorinated benzothiadiazole heterojunctions were constructed and the photophysical processes were investigated with femtosecond transient absorption spectroscopy. Encouragingly, an interfacial charge-transfer signal was detected in the spectra of the heterojunction, which provides solid evidence for S-scheme charge transfer to complement the results from well-established methods. Furthermore, the lifetime for interfacial charge transfer was calculated to be ca. 78.6 ps. Moreover, the S-scheme heterojunction photocatalysts exhibit higher photocatalytic conversion of 1,2-diols and H 2 production rates than bare cadmium sulfide.

关键词： 1,2-Diols Oxidation Hydrogen Production Photocatalysis S-Scheme Transient Absorption

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Frontispiece: Anion Modulation of Pt-Group Metals and Electrocatalysis Applications

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Chemistry – A European Journal 2021年第48期27卷

作者： Ding Chen Jiawei Zhu Dr. Zonghua Pu Prof. Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Foshan Xianhu Laboratory of Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China

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NH4+Deprotonation at Interfaces Induced Reversible H3O+/NH4+Co-insertion/Extraction

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Angewandte Chemie 2023年第14期135卷

作者： Meng Huang Qiu He Junjun Wang Xiong Liu Fangyu Xiong Yu Liu Ruiting Guo Yan Zhao Jinlong Yang Liqiang Mai Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen 518060 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China College of Materials Science and Engineering Sichuan University Chengdu 610065 China School of Materials Science and Engineering Zhengzhou University Zhengzhou 450001 China Department of Physics City University of Hong Kong Tat Chee Avenue Kowloon 999077 Hong Kong China Department of Materials Science and Engineering National University of Singapore Singapore 117574 Singapore The Institute of Technological Sciences Wuhan University Hubei Wuhan 430072 China

Ion insertions always involve electrode-electrolyte interface process, desolvation for instance, which determines the electrochemical kinetics. However, it′s still a challenge to achieve fast ion insertion and investigate ion transformation at interface. Herein, the interface deprotonation of NH 4 + and the introduced dissociation of H 2 O molecules to provide sufficient H 3 O + to insert into materials′ structure for fast energy storages are revealed. Lewis acidic ion-NH 4 + can, on one hand provide H 3 O + itself via deprotonation, and on the other hand hydrolyze with H 2 O molecules to produce H 3 O + . In situ attenuated total reflection-Fourier transform infrared ray method probed the interface accumulation and deprotonation of NH 4 + , and density functional theory calculations manifested that NH 4 + tend to thermodynamically adsorb on the surface of monoclinic VO 2 , and deprotonate to provide H 3 O + . In addition, the inserted NH 4 + has a positive effect for stabilizing the VO 2 (B) structure. Therefore, high specific capacity (>300 mAh g −1 ) and fast ionic insertion/extraction (<20 s) can be realized in VO 2 (B) anode. This interface derivation proposes a new path for designing proton ion insertion/extraction in mild electrolyte.

关键词： Electrode-Electrolyte Interface Energy Storage Mechanism Proton Insertion Vanadium Dioxide In Situ Characterization

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Hierarchical Zeolite Single-Crystal Reactor for Excellent Catalytic Efficiency

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Matter 2020年第4期3卷 1226-1245页

作者： Ming-Hui Sun Jian Zhou Zhi-Yi Hu Li-Hua Chen Li-Yuan Li Yang-Dong Wang Zai-Ku Xie Stuart Turner Gustaaf Van Tendeloo Tawfique Hasan Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 5000 Namur Wallonia Belgium State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Shanghai Research Institute of Petrochemical Technology SINOPEC Shanghai 201208 China Nanostructure Research Centre (NRC) Wuhan University of Technology Wuhan 430070 Hubei China Electron Microscopy for Materials Science (EMAT) University of Antwerp 2020 Antwerp Flemish Region Belgium Cambridge Graphene Centre University of Cambridge Cambridge CB3 0DS UK Clare Hall University of Cambridge Cambridge CB2 1EW UK

As a size- and shape-selective catalyst, zeolites are widely used in petroleum and fine-chemicals processing. However, their small micropores severely hinder molecular diffusion and are sensitive to coke formation. Hierarchically porous zeolite single crystals with fully interconnected, ordered, and tunable multimodal porosity at macro-, meso-, and microlength scale, like in leaves, offer the ideal solution. However, their synthesis remains highly challenging. Here, we report a versatile confined zeolite crystallization process to achieve these superior properties. Such zeolite single crystals lead to significantly improved mass transport properties by shortening the diffusion length while maintaining shape-selective properties, endowing them with a high efficiency of zeolite crystals, enhanced catalytic activities and lifetime, highly reduced coke formation, and reduced deactivation rate in bulky-molecule reactions and methanol-to-olefins process. Their industrial utilization can lead to the design of innovative and intensified reactors and processes with highly enhanced efficiency and minimum energy consumption.

关键词： MAP4: Demonstrate hierarchical zeolites zeolite single crystals ordered structure interconnected pores improved diffusion rate highly reduced coking catalytic efficiency catalytic cracking MTO process

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The enhanced dyes removal and catalytic property for nanofused structural chromium-benzenedicarboxylate metal-organic framework

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Chemical Physics Letters 2022年 803卷

作者： Tian Zhao Wei Geng Ming Dong Yi Zhao Christoph Janiak Ling Shen Jie Ying Xiao-Yu Yang School of Chemical Engineering and Technology Sun Yat-sen University Zhuhai 519082 China Hunan University of Technology Zhuzhou 412007 China Institut für Anorganische Chemie und Strukturchemie Heinrich-Heine-Universität Düsseldorf Universitätsstr. 1 D-40225 Düsseldorf Germany State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & Shenzhen Research Institute & Joint Laboratory for Marine Advanced Materials in Pilot National Laboratory for Marine Science and Technology (Qingdao) Wuhan University of Technology Wuhan 430070 China

MIL-101(Cr) can be tailored by using different modulators in the synthesis to obtain several morphological variants, including micro-sized MIL-101(Cr) (M-MIL), nano-sized MIL-101(Cr) (N-MIL) and nanofused hierarchical porous MIL-101(Cr) (H-MIL). Though those MILs had comparable porosity, H-MIL possessed remarkable higher adsorption capacity toward the anionic dye Congo red (CR, 1467 mg/g) and cationic dye methylene blue (MB, 301 mg/g) than the other two samples. Furthermore, in the cyanosilylation reaction, H-MIL also revealed significantly enhanced catalytic activity (yield ∼ 95.1%). Thus, the outstanding performance of H-MIL could be attributed to its hierarchically porous structure which accelerated the mass transfer rate and exposed more catalytic active sites.

关键词： Nanofused hierarchical porous MIL-101 Morphology control Dye adsorption Enhanced catalytic property MIL materials of Institute Lavoisier

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An oxygen-deficient vanadium oxide@N-doped carbon heterostructure for sodium-ion batteries: insights into the charge storage mechanism and enhanced reaction kinetics

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Journal of materials Chemistry A 2020年第6期8卷 3450-3458页

作者： Qingyuan Ren Ning Qin Bin Liu Yuan Yao Xu Zhao Zhao Deng Yu Li Yucheng Dong Dong Qian Bao-Lian Su Wenjun Zhang Hong-En Wang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan China Department of Materials Science and Technology Southern University of Science and Technology (SUSTC) Shenzhen China Centre of Super Diamond & Advanced Films (COSDAF) Department of Materials Science and Engineering City University of Hong Kong HKSAR China Beijing National Laboratory of Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China Institute of Chemical Materials Chinese Academy of Engineering Physics Mianyang 621900 China College of Chemistry and Chemical Engineering Central South University Changsha 410083 China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Belgium College of Physics and Electronics Information Yunnan Normal University Kunming 650500 China

Vanadium oxides are a class of promising anode candidates for sodium-ion batteries (SIBs) with high theoretical capacity and low cost. However, their practical application has been impeded by the low electronic conductivity, sluggish ionic transport and large volume change upon sodiation. Herein, a novel, high-performance anode for SIBs based on an oxygen-deficient vanadium oxide (VO/V₂O₃) heterostructure embedded in porous nitrogen-doped carbon (denoted as VNC) derived by a very simple and localized phase transition from a vanadium glycolate precursor has been demonstrated. The strong synergy of the hierarchically porous framework, VO/V₂O₃ phase heterojunctions with oxygen vacancy defects, and interfacial coupling with N-doped carbon (NC) efficiently promotes the electron/ion transport and alleviates the volume change during the sodiation/de-sodiation process. Electrochemical evaluation reveals that this novel VNC anode material manifests high sodium-ion storage capability and stability. Ex situ X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analyses show that (a portion of) the vanadium oxides can be converted into vanadium metal and sodium oxides. First-principles density functional theory (DFT) calculations reveal that coupling with NC effectively enhances the interfacial interactions and charge transfer between vanadium oxides and carbon, as well as the conversion reaction kinetics during sodiation/desodiation. The present work offers a viable strategy for the rational design and exploration of novel heterostructure composite electrodes for a wide array of beyond-lithium-ion batteries.

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Selective CO2Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Shenghua Chen Dr. Chengliang Ye Dr. Ziwei Wang Dr. Peng Li Dr. Wenjun Jiang Dr. Zechao Zhuang Dr. Jiexin Zhu Dr. Xiaobo Zheng Dr. Shahid Zaman Dr. Honghui Ou Lei Lv Dr. Lin Tan Dr. Yaqiong Su Dr. Jiang Ouyang Prof. Dingsheng Wang National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology School of Chemical Engineering and Technology Xi'an Jiaotong University Xi'an 710049 P. R. China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 P. R. China School of Chemistry Xi'an Key Laboratory of Sustainable Energy Materials Chemistry State Key Laboratory of Electrical Insulation and Power Equipment Engineering Research Center of Energy Storage Materials and Devices Ministry of Education Xi'an Jiaotong University Xi'an 710049 P. R. China Qian Xuesen Laboratory of Space Technology China Academy of Space Technology Beijing 100094 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 P. R China Key Laboratory of Energy Conversion and Storage Technologies Department of Mechanical and Energy Engineering Southern University of Science and Technology Shenzhen 518055 P. R. China School of Biomedical Engineering Guangzhou Medical University Guangzhou 511436 P. R. China

Electrochemical CO 2 reduction reaction (CO 2 RR) over Cu catalysts exhibits enormous potential for efficiently converting CO 2 to ethylene (C 2 H 4 ). However, achieving high C 2 H 4 selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CO 2 RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating the reconstruction of a Cu-based material to a pathway that facilitates CO 2 reduction to C 2 H 4 products. An excellent Faraday efficiency (FE) of 63.6 % on C 2 H 4 with a current density of 497.2 mA cm −2 in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH 4 . The in situ X-ray absorption spectroscopy and Raman studies reveal that the hydroxyl group in TA stabilizes Cu δ+ during the CO 2 RR. Furthermore, theoretical calculations demonstrate that the Cu δ+ /Cu 0 interfaces lower the activation energy barrier for *CO dimerization, and hydroxyl species stabilize the *COH intermediate via hydrogen bonding, thereby promoting C 2 H 4 production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO 2 reduction to value-added chemicals.

关键词： C2H4 CO2RR Cuδ+/Cu0 Hydrogen Bonding TA Molecule

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