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A Supramolecular Complex of C60–S with High-Density Active Sites as a Cathode for Lithium–Sulfur Batteries

Angewandte Chemie 2021年第26期133卷

作者： Jingwei Xiang Wangqiang Shen Zezhou Guo Jintao Meng Prof. Lixia Yuan Yi Zhang Zexiao Cheng Prof. Yue Shen Prof. Xing Lu Prof. Yunhui Huang State Key Laboratory of Material Processing and Die and Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China

The well-known “shuttle effect” of the intermediate lithium polysulfides (LiPSs) and low sulfur utilization hinder the practical application of lithium–sulfur (Li–S) batteries. Herein, we describe a novel C 60 –S supramolecular complex with high-density active sites for LiPS adsorption that was formed by a simple one-step process as a cathode material for Li–S batteries. Benefiting from the cocrystal structure, 100 % of the C 60 molecules in the complex can offer active sites to adsorb LiPSs and catalyze their conversion. Furthermore, the lithiated C 60 cores promote internal ion transport inside the composite cathode. At a low electrolyte/sulfur ratio of 5 μL mg −1 , the C 60 –S cathode with a sulfur loading of 4 mg cm −2 exhibited a high capacity of 809 mAh g −1 (3.2 mAh cm −2 ). The development of the C 60 –S supramolecular complex will inspire the invention of a new family of S/fullerenes as cathodes for high-performance Li–S batteries and extend the application of fullerenes.

关键词： fullerenes high-density active sites lithium–sulfur batteries shuttle effect supramolecular complexes

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Delocalized Isoelectronic Heterostructured FeCoO_xS_y Catalysts with Tunable Electron Density for Accelerated Sulfur Redox Kinetics in Li-S batteries

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Angewandte Chemie - International Edition 2023年第47期62卷 e202311693-e202311693页

作者： Chen, Peng Wang, Tianyi He, Di Shi, Ting Chen, Manfang Fang, Kan Lin, Hongzhen Wang, Jian Wang, Chengyin Pang, Huan Institute for Innovative Materials and Energy Faculty of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 China i-Lab and CAS Key Laboratory of Nanophotonic Materials and Devices Suzhou Institute of Nano-tech and Nano-bionics Chinese Academy of Sciences Suzhou 215123 China Helmholtz Institute Ulm (HIU) Ulm D-89081 Germany State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China National Base for International Science & Technology Cooperation School of Chemistry Xiangtan University Xiangtan 411105 China School of Materials Science and Engineering Harbin Institute of Technology (Shenzhen) Shenzhen 518055 China

High interconversion energy barriers, depressive reaction kinetics of sulfur species, and sluggish Li+ transport inhibit the wide development of high-energy-density lithium sulfur (Li−S) batteries. Herein, differing f... 详细信息

High interconversion energy barriers, depressive reaction kinetics of sulfur species, and sluggish Li⁺ transport inhibit the wide development of high-energy-density lithium sulfur (Li−S) batteries. Herein, differing from random mixture of selected catalysts, the composite catalyst with outer delocalized isoelectronic heterostructure (DIHC) is proposed and optimized, enhancing the catalytic efficiency for decreasing related energy barriers. As a proof-of-content, the FeCoO_xS_y composites with different degrees of sulfurization are fabricated by regulating atoms ratio between O and S. The relationship of catalytic efficiency and principal mechanism in DIHCs are deeply understood from electrochemical experiments to in situ/operando spectral spectroscopies i.e., Raman, XRD and UV/Vis. Consequently, the polysulfide conversion and Li₂S precipitation/dissolution experiments strongly demonstrate the volcano-like catalytic efficiency of various DIHCs. Furthermore, the FeCoO_xS_y-decorated cell delivers the high performance (1413 mAh g⁻¹ at 0.1 A g⁻¹). Under the low electrolyte/sulfur ratio, the high loading cell stabilizes the areal capacity of 6.67 mAh cm⁻² at 0.2 A g⁻¹. Impressively, even resting for about 17 days for possible polysulfide shuttling, the high-mass-loading FeCoO_xS_y-decorated cell stabilizes the same capacity, showing the practical application of the DIHCs in improving catalytic efficiency and reaching high electrochemical performance. © 2023 Wiley-VCH GmbH.

关键词： Adsorption and Catalytic Delocalized Isoelectronic Heterostructure Catalyst in-Situ Characterization Iso-e S and O Lithium Sulfur Battery

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Hierarchical aging pathways and signatures of thermodynamic transition in molecular glasses

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Science China materials 2019年第6期62卷 864-872页

作者： Shiyu Liu Yao Yu Lin Liu Yue Wu School of Materials Science and Engineering and State Key Lab for Materials Processing and Die and Mold Technology Huazhong University of Science and Technology Wuhan National High Magnetic Field Center Huazhong University of Science and Technology Department of Physics and Astronomy University of North Carolina at Chapel Hill

When a liquid is supercooled,its structural equilibration timeτeqincreases sharply approaching the glass transition temperature Tg,below which it is kinetically arrested in the out of equilibrium glassy *** annealing below Tg,such glassy state relaxes toward the equilibrium *** is growing evidence that such relaxation process is quite complex,influenced by the complexity of the potential energy *** we report the observation of a hierarchical aging pathway in the process of the glass-to-supercooled liquid transition in various molecular glass forming *** scanning calorimetry reveals that the glassy state upon annealing below Tgfirstly enters a transient metastable supercooled liquid state with slightly higher enthalpies than that of the equilibrium supercooled liquid state when extrapolated to below *** observation is also confirmed by structural measurements via Raman *** dynamics of the transient metastable-to-stable supercooled liquid transition exhibits characteristics of thermodynamic transition at spinodal temperature Tspslightly above Tg,leading to anomalous behaviors such as the appearance of a transition-like behavior in the plot of fragility *** observations imply that the free energy landscape of the supercooled liquid develops complexity with qualitative changes approaching Tgand could have strong influence on the process of the glass transition.

关键词： glass transition hierarchical aging pathways thermodynamic transition metastability

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Lithium-Metal Batteries: Polycationic Polymer Layer for Air-Stable and Dendrite-Free Li Metal Anodes in Carbonate Electrolytes (Adv. Mater. 12/2021)

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Advanced materials 2021年第12期33卷

作者： Jingyi Wu Zhixiang Rao Xueting Liu Yue Shen Chun Fang Lixia Yuan Zhen Li Wuxing Zhang Xiaolin Xie Yunhui Huang State Key Laboratory of Material Processing and Die & Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China Key Laboratory of Material Chemistry for Energy Conversion and Storage School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China

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Lithium Metal Anodes: Composite Lithium Metal Anodes with Lithiophilic and Low-Tortuosity Scaffold Enabling Ultrahigh Currents and Capacities in Carbonate Electrolytes (Adv. Funct. Mater. 14/2021)

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Advanced Functional materials 2021年第14期31卷

作者： Jingyi Wu Zhixiang Rao Xueting Liu Yue Shen Lixia Yuan Zhen Li Xiaolin Xie Yunhui Huang State Key Laboratory of Material Processing and Die & Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China Key Laboratory of Material Chemistry for Energy Conversion and Storage School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China

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Ultrathin Conductive Interlayers: Ultrathin Conductive Interlayer with High-Density Antisite Defects for Advanced Lithium–Sulfur Batteries (Adv. Funct. Mater. 2/2021)

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Advanced Functional materials 2021年第2期31卷

作者： Danqi He Jintao Meng Xinyu Chen Yaqi Liao Zexiao Cheng Lixia Yuan Zhen Li Yunhui Huang State Key Laboratory of Material Processing and Die & Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China College of Materials Science and Engineering Beijing University of Chemical Technology Beijing 100029 China

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Enhancing Microdomain Consistency in Polymer Electrolytes towards Sustainable Lithium Batteries

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Angewandte Chemie 2024年第5期137卷

作者： Dr. Yang Feng Dr. Yanpeng Fan Dr. Lingfei Zhao Dr. Jiangtao Yu Dr. Yaqi Liao Dr. Tongrui Zhang Ruochen Zhang Dr. Haitao Zhu Dr. Xingwei Sun Prof. Zhe Hu Prof. Kai Zhang Prof. Jun Chen State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) College of Chemistry Nankai University Tianjin 300071 China Institute for Superconducting & Electronic Materials University of Wollongong Innovation Campus Squires Way North Wollongong NSW 2500 Australia State Key Laboratory of Material Processing and Die and Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192 China

Polymer electrolytes incorporated with fillers possess immense potential for constructing the fast and selective Li + conduction. However, the inhomogeneous distribution of the fillers usually deteriorates the microdomain consistency of the electrolytes, resulting in uneven Li + flux, and unstable electrode-electrolyte interfaces. Herein, we formulate a solution-process chemistry to in situ construct gel polymer electrolytes (GPEs) with well-dispersed metal–organic frameworks (MOFs), leading to a uniform microdomain structure. Through the integration of X-ray computed tomography analyses and theoretical simulations, our research identifies that the improvement of microdomain consistency in GPEs is beneficial for enhancing its mechanical strength, homogenizing ionic/electronic field distribution and upgrading the interface stability with the elctrodes. Moreover, consistently spread MOFs bind effectively with Lewis-base anions of Li salts, enhancing Li + kinetics. Owing to these advantages, the developed GPEs achieve a high conductivity of 1.51 mS cm −1 and a Li + transference number of 0.66, resulting in exceptional cyclab.lity of lithium metal electrodes (over 1800 hours). Additionally, the solid-state NCM811//Li pouch batteries exhibit an impressive capacity retention of 94.2 % over 200 cycles with an N/P ratio of 1.69. This study emphasizes the significant impact of microdomain structural chemistry on the advancement of solid-state batteries.

关键词： Microdomain structure Metal–organic frameworks Gel polymer electrolytes Lithium deposition Lithium-metal batteries

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Effect of laser energy density on transformation behavior and mechanical property of NiTi alloys fabricated by laser powder bed fusion

Smart Manufacturing

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Smart Manufacturing 2022年第2期1卷

作者： Xiaoqiang Wang Yakun Tao Shifeng Wen Yan Zhou Yusheng Shi State Key Laboratory of Material Processing and Die & Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 P. R. China Faculty of Engineering China University of Geosciences Wuhan 430074 P. R. China School of Civil and Hydraulic Engineering National Center of Technology Innovation for Digital Construction Huazhong University of Science and Technology Wuhan 430074 P. R. China

This research investigated the influence of laser energy density on the phase transformation characteristics and structure, together with the mechanical property of NiTi shape memory alloys fabricated by laser powder bed fusion (LPBF). Results showed that randomly oriented needle-shaped martensite was distributed in the B2 austenite matrix in samples with the higher energy density. In contrast, typical columnar grains were observed throughout multiple melt pools, showing obvious epitaxial growth characteristics in the samples with lower energy density. Besides, the martensite transformation temperature varied approximately linearly with the increasing laser energy density, showing a positive correlation. It can be explained that more intense evaporation of Ni element in the melt pool under higher energy density leads to a reduction in the Ni content of the matrix and contributes to a reduction in the lattice distortion of the B2 matrix. Finally, the samples with the energy density of 138.89 J/mm 3 showed optimal tensile and compression strength of 648 and 2970 MPa, respectively. This work provides a novel approach to optimize the performance of LPBF NiTi sample by tailoring the phase composition and structure through the laser energy density.

关键词： Laser powder bed fusion (LPBF) NiTi shape memory alloys transformation temperature laser energy density phase composition and structure

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Observation of the out-of-plane polarized spin current from CVD grown WTe2

arXiv

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arXiv 2021年

作者： Shi, Shuyuan Li, Jie Hsu, Chuang-Han Lee, Kyusup Wang, Yi Yang, Li Wang, Junyong Wang, Qisheng Wu, Hao Zhang, Wenfeng Eda, Goki Liang, Gengchiau Chang, Haixin Yang, Hyunsoo Department of Electrical and Computer Engineering National University of Singapore 117576 Singapore Quantum-Nano Matter and Device Lab State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan430074 China Institute of Physics Academia Sinica Taipei11529 Taiwan Key Laboratory of Materials Modification by Laser Ion and Electron Beams Ministry of Education Dalian University of Technology Dalian116024 China Centre for Advanced 2D Materials National University of Singapore 6 Science Drive 2 117546 Singapore Department of Physics National University of Singapore 117542 Singapore

Weyl semimetal Td-phase WTe2 possesses the spin-resolved band structure with strong spin-orbit coupling, holding promises as a useful spin source material. The noncentrosymmetric crystalline structure of Td-WTe2 endows the generation of the out-of-plane polarized spin, which is of great interest in magnetic memory applications. Previously, WTe2 was explored in spin devices based on mechanically exfoliated single crystal flakes with a size of micrometers. For practical spintronics applications, it is highly desirable to implement wafer-scale thin films. In this work, we utilize centimeter-scale chemical vapor deposition (CVD)-grown Td-WTe2 thin films and study the spin current generation by the spin torque ferromagnetic resonance technique. We find the in-plane and out-of-plane spin conductivities of 7.36 × 103 (ħ/2e) (Ωm)–1 and 1.76 × 103 (ħ/2e) (Ωm)–1, respectively, in CVD-growth 5 nm-WTe2. We further demonstrate the current induced magnetization switching in WTe2/NiFe at room temperature in the domain wall motion regime, which may invigorate potential spintronic device innovations based on Weyl semimetals. Copyright © 2021, The Authors. All rights reserved.

关键词： Thin films

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Vacancy-Rich Ni(OH)2 Drives the Electrooxidation of Amino C−N Bonds to Nitrile C≡N Bonds

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Angewandte Chemie 2020年第39期132卷

作者： Wang W. Wang Y. Yang R. Wen Q. Liu Y. Jiang Z. Li H. Zhai T. State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China

Electrochemical synthesis based on electrons as reagents provides a broad prospect for commodity chemical manufacturing. A direct one-step route for the electrooxidation of amino C−N bonds to nitrile C≡N bonds offers an alternative pathway for nitrile production. However, this route has not been fully explored with respect to either the chemical bond reforming process or the performance optimization. Proposed here is a model of vacancy-rich Ni(OH)2 atomic layers for studying the performance relationship with respect to structure. Theoretical calculations show the vacancy-induced local electropositive sites chemisorb the N atom with a lone pair of electrons and then attack the corresponding N(sp3)−H, thus accelerating amino C−N bond activation for dehydrogenation directly into the C≡N bond. Vacancy-rich nanosheets exhibit up to 96.5 % propionitrile selectivity at a moderate potential of 1.38 V. These findings can lead to a new pathway for facilitating catalytic reactions in the chemicals industry. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

关键词： amines electrochemistry nanostructures oxidation surface chemistry

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