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A Bifunctional CdS/MoO2/MoS2Catalyst Enhances Photocatalytic H2Evolution and Pyruvic Acid synthesis

Angewandte Chemie 2022年第44期134卷

作者： Dr. Chuanbiao Bie Dr. Bicheng Zhu Dr. Linxi Wang Prof. Huogen Yu Dr. Chenhui Jiang Prof. Tao Chen Prof. Jiaguo Yu Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 430074 Wuhan P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 430070 Wuhan P. R. China Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China 230026 Hefei P. R. China

The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst is constructed based on CdS/MoO 2 /MoS 2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic acid (LA) oxidation. MoS 2 and MoO 2 are simultaneously obtained from the conversion of CdMoO 4 in one step. In a photocatalytic process, the MoS 2 and MoO 2 function as the reduction and oxidation centers on which photogenerated electrons and holes accumulate and are used for hydrogen evolution reaction (HER) and PA synthesis, respectively. By monitoring the intermediates, a two-step single-electron route for PA production is proposed, initiated by the cleavage of the α-C(sp 3 )−H bond in the LA. The conversion of LA and the selectivity of PA can reach ca . 29 % and 95 % after a five-hour reaction, respectively.

关键词： CdS Dual Cocatalysts Hollow Sphere Hydrogen Evolution Organic synthesis

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The Nucleation Process in the Preparation of Graphene Films by Pulsed Laser Deposition

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Journal of Wuhan University of technology(materials Science) 2018年第2期33卷 343-348页

作者：王进 WANG Xuemin YU Jian XIAO Tingting PENG Liping XIONG Zhengwei CAO Linhong WANG Chuanbin 沈强 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Research Center of Laser Fusion China Academy of Engineering Physics Laboratory for Extreme Conditions Matter Properties Southwest University of Science and Technology School of Materials Science and Engineering Southwest University of Science and Technology

The nucleation process of graphene films prepared by pulsed laser deposition has been investigated in detail. It is found that graphene nucleates at the steps on the substrate surface firstly, from aggregation of nuclei into particles. High pulsed laser energy offers large incident energy for carbon particles deposited on the surface of the substrate, which is beneficial to the nucleation of graphene. A lot of steps are formed on the copper substrate due to the high temperature, so that the high incident energetic carbon species are able to form a stable nucleus at the steps. As the incident particles increases, the graphene nuclei are combined to grow together. Further, it is found that graphene tends to form few layer graphene particles instead of large graphene sheets.

关键词： graphene PLD nucleation

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Enhanced Carrier Diffusion Enables Efficient Back-Contact Perovskite Photovoltaics

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Angewandte Chemie 2023年第27期135卷

作者： Boya Zhao Dr. Lara V. Gillan Dr. Andrew D. Scully Dr. Anthony S. R. Chesman Dr. Boer Tan Dr. Xiongfeng Lin Dr. Jingying Liu Dr. Kevin J. Rietwyk Siqi Deng Dr. Christopher Bailey Prof. Yi-Bing Cheng Prof. Dane R. McCamey Prof. Udo Bach Department of Chemical and Biological Engineering Monash University Victoria 3800 Australia ARC Centre of Excellence in Exciton Science Australia School of Physics University of New South Wales New South Wales 2052 Australia CSIRO Manufacturing Victoria 3168 Australia Department of Materials Science and Engineering Monash University Victoria 3800 Australia State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Foshan Xianhu Laboratory Foshan 528216 China

Back-contact architectures offer a promising route to improve the record efficiencies of perovskite solar cells (PSCs) by eliminating parasitic light absorption. However, the performance of back-contact PSCs is limited by inadequate carrier diffusion in perovskite. Here, we report that perovskite films with a preferred out-of-plane orientation show improved carrier dynamic properties. With the addition of guanidine thiocyanate, the films exhibit carrier lifetimes and mobilities increased by 3–5 times, leading to diffusion lengths exceeding 7 μm. The enhanced carrier diffusion results from substantial suppression of nonradiative recombination and improves charge collection. Devices using such films achieve reproducible efficiencies reaching 11.2 %, among the best performances for back-contact PSCs. Our findings demonstrate the impact of carrier dynamics on back-contact PSCs and provide the basis for a new route to high-performance back-contact perovskite optoelectronic devices at low cost.

关键词： Back-Contact Architecture Carrier Dynamics Crystallographic Orientation Guanidine Thiocyanate Perovskite Solar Cells

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Reversible Zn Metal Anodes Enabled by Trace Amounts of Underpotential Deposition Initiators

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Angewandte Chemie 2023年第18期135卷

作者： Yuhang Dai Chengyi Zhang Wei Zhang Lianmeng Cui Chumei Ye Xufeng Hong Jinghao Li Ruwei Chen Wei Zong Xuan Gao Jiexin Zhu Peie Jiang Qinyou An Prof. Dan J. L. Brett Prof. Ivan P. Parkin Dr. Guanjie He Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Christopher Ingold Laboratory Department of Chemistry University College London London WC1H 0AJ UK Electrochemical Innovation Lab Department of Chemical Engineering University College London London WC1E 7JE UK Institute of Technological Sciences Wuhan University Wuhan 430072 P. R. China Department of Materials Science and Metallurgy University of Cambridge Cambridge CB3 0FS UK Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials School of Materials Science and Engineering Peking University Beijing 100871 P. R. China

Routine electrolyte additives are not effective enough for uniform zinc (Zn) deposition, because they are hard to proactively guide atomic-level Zn deposition. Here, based on underpotential deposition (UPD), we propose an “escort effect” of electrolyte additives for uniform Zn deposition at the atomic level. With nickel ion (Ni 2+ ) additives, we found that metallic Ni deposits preferentially and triggers the UPD of Zn on Ni. This facilitates firm nucleation and uniform growth of Zn while suppressing side reactions. Besides, Ni dissolves back into the electrolyte after Zn stripping with no influence on interfacial charge transfer resistance. Consequently, the optimized cell operates for over 900 h at 1 mA cm −2 (more than 4 times longer than the blank one). Moreover, the universality of “escort effect” is identified by using Cr 3+ and Co 2+ additives. This work would inspire a wide range of atomic-level principles by controlling interfacial electrochemistry for various metal batteries.

关键词： Aqueous Battery Electrolyte Additive Interfacial Electrochemistry Underpotential Deposition Zinc Anode

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Bifunctional o-CoSe 2 /c-CoSe 2 /MoSe 2 heterostructures for enhanced electrocatalytic and photoelectrochemical hydrogen evolution reaction

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materials Today Chemistry 2022年 23卷

作者： Y. Ji W. Luo Y. Liu Z. He N. Cheng Z. Zhang X. Qi J. Zhong L. Ren Hunan Key Laboratory of Micro-Nano Energy Materials and Devices Laboratory for Quantum Engineering and Micro-Nano Energy Technology Faculty of Materials and Optoelectronic Physics Xiangtan University Hunan 411105 PR China Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Institutes of Physical Science and Information Technology Anhui University Hefei 230601 PR China Department of Materials Science and Engineering and Shenzhen Key Laboratory of Hydrogen Energy Southern University of Science and Technology Shenzhen 518055 PR 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 PR China

The bottleneck of alkaline hydrogen evolution reaction lies in the kinetically sluggish brought from multistep reaction processes involving water adsorption and dissociation, as well as hydrogen adsorption. In this work, we successfully synthesized o-CoSe 2 /c-CoSe 2 heterostructures anchored on MoSe 2 nanosheets to powerfully promote reaction processes. As an electrocatalyst, it exhibits a low overpotential of 112 mV at 10 mA/cm 2 and a Tafel slope of 96.9 mV/dec for an alkaline hydrogen evolution reaction. Moreover, the as-prepared catalyst can behave as both cathode and anode for overall water splitting, which only requires 1.61 V cell voltage at 10 mA/cm 2 . Significantly, the cell voltage can be further reduced to 1.53 V at 10 mA/cm 2 for water electrolysis under the simulated solar irradiation owing to such a semiconductor-based heterostructure that facilitates the separation of photogenerated charges. Here, the improving overall performance of this ternary electrocatalyst is attributed to the multifunctionality and synergistic interaction of different components in this heterogeneous material. The work provides a novel strategy to design active catalysts simultaneously using electric energy and solar energy for effective water splitting.

关键词： Transition-metal dichalcogenides Ternary hybrids Alkaline hydrogen evolution Photoelectrochemical water splitting

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Ultrathin nanobelts-assembled Chinese knot-like 3D TiO2 for fast and stable lithium storage

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Nano Research 2018年第4期11卷 2116-2128页

作者： Qili Wu Shiman He Xianfeng Yang Jingling Yang Gaoren Li Yuying Meng Shengfu Tong Liqiang Mai Mingmei Wu MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-Sen University Guangzhou 510275 China Analytical and Testing Center South China University of Technology Guangzhou 510640 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China

Nanostructured TiO2 has applications in solar cells, photocatalysts, and fast- charging, safe lithium ion batteries （LIBs）. To meet the demand of high-capacity and high-rate LIBs with TiO2-based anodes, it is important to fine-tune the nanoarchitecture using a well-controlled synthesis approach. Herein, we report a new approach that involves epitaxial growth combined with topotactic conversion to synthesize a unique type of three-dimensional （3D） TiO2 nano- architecture that is assembled by well-oriented ultrathin nanobelts. The whole nanoarchitecture displays a 3D Chinese knot-like morphology; the core consists of robust perpendicular interwoven nanobelts and the shell is made of extended nanobelts. The nanobelts oriented in three perpendicular [001]A directions facilitate Li＋ penetration and diffusion. Abundant anatase/TiO2-B interfaces provide a large amount of interfacial pseudocapacitance. A high and stable capacity of 130 mA.h.g-1 was obtained after 3,000 cycles at 10 A·g-1 （50 C）, and the high-rate property of our material was greater than that of many recently reported high-rate TiO2 anodes. Our result provides, not only a novel synthesis strategy, but also a new type of 3D anatase TiO2 anode that may be useful in developing long-lasting and fast-charging batteries.

关键词： three-dimensional （3D） nanoarchitectures ultrathin nanobelts TiO2 lithium ion storage ultrahigh rate battery

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Degradation of Silicone Rubbers in Fenton's Reagents

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Journal of Wuhan University of technology(materials Science) 2018年第4期33卷 793-796页

作者：吴凡李克 ZHANG Qinglian ZHANG Haining CHEN Yanan PAN Mu YAN Xinping State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology National Engineering Research Center for Waterway Transport Safety Intelligent Transport Systems Research Center Wuhan University of Technology Hubei Key Laboratory of Fuel Cells Wuhan University of Technology

Gaskets are applied in PEMFCs（proton exchange membrane fuel cells） to keep reactant gases and liquid within their respective regions, which are of great significance for the both sealing and electrochemical performance of fuel cells during the long-term operation. In this study, the degradation of silicone rubbers, often selected as seals in PEMFCs, in Fenton＇s reagents with different H_2O_2 concentrations was investigated. The changes in chemical properties, mechanical behavior and surface morphology of the samples were studied before and after exposure to the test environment over time. It is found that increasing H_2O_2 concentration will degrade the rubbers more severely. The experimental results elucidate the degradation mechanism of silicone rubbers in Fenton＇s reagents and the influence of H_2O_2 in the degradation process.

关键词： silicone rubbers PEMFCs seal degradation Fenton＇s reagents

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Structure of triplite LiFeSO 4F powder synthesized through an ambient two-step solid-state route

Structure of triplite LiFeSO 4F powder synthesized through a...

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作者： Ma, F.-F. Mao, J.-W. Shao, G.-Q. Fan, S.-H. Zhu, C. Zhang, A.-L. Xie, G.-Z. Gu, J.-N. Yan, J.-L. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan430070 China

The triplite LiFeSO4F displays both the highest potential ever reported for an Fe-based compound, as well as a comparable specific energy with that of popular LiFePO4. The synthesis is still a challenge because the present approaches are connected with long time, special equipments or organic reagents, etc. In this work, the triplite LiFeSO4F powder was synthesized through an ambient two-step solid-state route. The reaction process and phase purity were analyzed, coupled with structure refinement and electrochemical test. © Copyright International Centre for Diffraction Data 2018.

关键词： Iron compounds

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Unprecedented and highly stable lithium storage capacity of (001) faceted nanosheet-constructed hierarchically porous TiO2/rGO hybrid architecture for high-performance Li-ion batteries

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National science review 2020年第6期7卷 1046-1058页

作者： Wen-Bei Yu Zhi-Yi Hu Jun Jin Min Yi Min Yan Yu Li Hong-En Wang Huan-Xin Gao Li-Qiang Mai Tawfique Hasan Bai-Xiang Xu Dong-Liang Peng Gustaaf Van Tendeloo Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China. Institute of Materials Science Technische Universität Darmstadt Darmstadt 64287 Germany. Fundamental Research Department SINOPEC Shanghai Research Institute of Petrochemical Technology Shanghai 201208 China. Cambridge Graphene Centre University of Cambridge Cambridge CB3 0FA UK. Department of Materials Science and Engineering College of Materials Xiamen University Xiamen 361005 China. Nanostructure Research Centre Wuhan University of Technology Wuhan 430070 China.

Active crystal facets can generate special properties for various applications. Herein, we report a (001) faceted nanosheet-constructed hierarchically porous TiO/rGO hybrid architecture with unprecedented and highly stable lithium storage performance. Density functional theory calculations show that the (001) faceted TiO nanosheets enable enhanced reaction kinetics by reinforcing their contact with the electrolyte and shortening the path length of Li diffusion and insertion-extraction. The reduced graphene oxide (rGO) nanosheets in this TiO/rGO hybrid largely improve charge transport, while the porous hierarchy at different length scales favors continuous electrolyte permeation and accommodates volume change. This hierarchically porous TiO/rGO hybrid anode material demonstrates an excellent reversible capacity of 250 mAh g at 1 C (1 C = 335 mA g) at a voltage window of 1.0-3.0 V. Even after 1000 cycles at 5 C and 500 cycles at 10 C, the anode retains exceptional and stable capacities of 176 and 160 mAh g, respectively. Moreover, the formed LiTiO nanodots facilitate reversed Li insertion-extraction during the cycling process. The above results indicate the best performance of TiO-based materials as anodes for lithium-ion batteries reported in the literature.

关键词： (001) faceted TiO2 nanosheets Li2Ti2O4 crystallites porous hierarchy reduced graphene oxide unprecedented lithium storage capacity

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A High-Energy NASICON-Type Na3.2MnTi0.8V0.2(PO4)3Cathode Material with Reversible 3.2-Electron Redox Reaction for Sodium-Ion Batteries

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Angewandte Chemie 2023年第14期135卷

作者： Dr. Ping Hu Dr. Ting Zhu Congcong Cai Dr. Xuanpeng Wang Dr. Lei Zhang Prof. Liqiang Mai Prof. Liang Zhou Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Key Laboratory of Textile Fiber and Products Ministry of Education Hubei International Scientific and Technological Cooperation Base of Intelligent Textile Materials & Application Wuhan Textile University Wuhan 430200 China Department of Physical Science & Technology School of Science Wuhan University of Technology Luoshi Road 122 Wuhan 430070 P. R. China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 Hubei China

Na superionic conductor (NASICON) structured cathode materials with robust structural stability and large Na + diffusion channels have aroused great interest in sodium-ion batteries (SIBs). However, most of NASICON-type cathode materials exhibit redox reaction of no more than three electrons per formula, which strictly limits capacity and energy density. Herein, a series of NASICON-type Na 3+ x MnTi 1− x V x (PO 4 ) 3 cathode materials are designed, which demonstrate not only a multi-electron reaction but also high voltage platform. With five redox couples from V 5+/4+ (≈4.1 V), Mn 4+/3+ (≈4.0 V), Mn 3+/2+ (≈3.6 V), V 4+/3+ (≈3.4 V), and Ti 4+/3+ (≈2.1 V), the optimized material, Na 3.2 MnTi 0.8 V 0.2 (PO 4 ) 3 , realizes a reversible 3.2-electron redox reaction, enabling a high discharge capacity (172.5 mAh g −1 ) and an ultrahigh energy density (527.2 Wh kg −1 ). This work sheds light on the rational construction of NASICON-type cathode materials with multi-electron redox reaction for high-energy SIBs.

关键词： Cathode Material Multi-Electron Redox Reaction NASICON Structure Na3+xMnTi1−xVx(PO4)3 Sodium-Ion Batteries

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