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Multiscale Anion-Hybrid in Atomic Ni Sites for High-Rate Water Electrolysis: Insights into the Charge Accumulation Mechanism

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Journal of the American Chemical Society 2024年第20期146卷 14194-14202页

作者： Li, Yan Peng, Yanan Dong, Wenda Jiang, Xueyu Lu, Lijun Yang, Dali Hsu, Liang-Ching Li, Wu Su, Baolian Lei, Aiwen Wuhan University Hubei Wuhan430072 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China National Chung Hsing University Taichung40227 Taiwan

Single-atom catalysts, characterized by transition metal-(N/O)4 units on nanocarbon (M-(N/O)4-C), have emerged as efficient performers in water electrolysis. However, there are few guiding principles for accurately controlling the ligand fields of single atoms to further stimulate the catalyst activities. Herein, using the Ni-(N/O)4-C unit as a model, we develop a further modification of the P anion on the outer shells to modulate the morphology of the ligand. The catalyst thus prepared possesses high activity and excellent long-term durability, surpassing commercial Pt/C, RuO2, and currently reported single-atom catalysts. Notably, mechanistic studies demonstrated that the pseudocapacitive feature of multiscale anion-hybrid nanocarbon is considerable at accumulating enough positive charge [Q], contributing to the high oxygen evolution reaction (OER) order (β) through the rate formula. DFT calculations also indicate that the catalytic activity is decided by the suitable barrier energy of the intermediates due to charge accumulation. This work reveals the activity origin of single atoms on multihybrid nanocarbon, providing a clear experiential formula for designing the electronic configuration of single-atom catalysts to boost electrocatalytic performance. © 2024 American Chemical Society.

关键词： Catalyst activity

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A flame-retardant binder with high polysulfide affinity for safe and stable lithium–sulfur batteries

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Science China Chemistry 2024年第3期67卷 1028-1036页

作者： Guowei Yu Guofeng Ye Cheng Wang Chenyang Wang Zhaoyun Wang Pu Hu Yu Li Xi-Xi Feng Shuang-Jie Tan Min Yan Sen Xin Zhitian Liu Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Hubei Engineering Technology Research Center of Optoelectronic and New Energy MaterialsSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.

关键词： lithium–sulfur battery polymer binder polysulfide affinity flame retardancy

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Serrated lithium fluoride nanofibers-woven interlayer enables uniform lithium deposition for lithium-metal batteries

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National Science Review 2022年第11期9卷 194-207页

作者： Shuangshuang Tan Yalong Jiang Shuyan Ni Hao Wang Fangyu Xiong Lianmeng Cui Xuelei Pan Chen Tang Yaoguang Rong Qinyou An Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology College of Materials Science and Engineering Chongqing University Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory

The uncontrollable formation of Li dendrites has become the biggest obstacle to the practical application of Li-metal anodes in high-energy rechargeable Li batteries. Herein, a unique LiF interlayer woven by millimeter-level, single-crystal and serrated LiF nanofibers（NFs） was designed to enable dendrite-free and highly efficient Li-metal deposition. This high-conductivity Li F interlayer can increase the Li+transference number and induce the formation of 'Li F–NFs-rich' solid–electrolyte interface（SEI）. In the 'Li F–NFs-rich'SEI, the ultra-long Li F nanofibers provide a continuously interfacial Li+transport path. Moreover, the formed Li–LiF interface between Li-metal and SEI film renders low Li nucleation and high Li+migration energy barriers, leading to uniform Li plating and stripping processes. As a result, steady charge–discharge in a Li//Li symmetrical cell for 1600 h under 4 m Ah cm-2and 400 stable cycles under a high area capacity of 5.65 mAh cm-2in a high-loading Li//rGO–S cell at 17.9 mA cm-2could be achieved. The free-standing LiF –NFs interlayer exhibits superior advantages for commercial Li batteries and displays significant potential for expanding the applications in solid Li batteries.

关键词： lithium fluoride serrated nanofibers LiF interlayer uniform Li deposition lithium-metal batteries

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Reduced graphene oxide-induced in-situ uniform growth of hydrated WO_(3) film for enhanced electrochromic performance

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Nano Research 2025年第4期18卷 569-577页

作者： Rui Fang Yang Liu Chunyu Shi Huihui Jin Zibo Chen Haohao Sun Ben Lv Daping He Xusheng Zheng Yuli Xiong State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China School of Science Wuhan University of TechnologyWuhan 430070China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

WO_(3)-graphene electrochromic materials are widely used in electrochromic devices including smart windows and electronic displays,due to their ability to adjust optical transmittance in the visible and near-infrared ranges under low electrode ***,the uniformity of the film remains a challenge for the widely used physical mixing-coating *** this study,we present a two-dimensional material-assisted synthesis of a porous hydrated WO_(3) film(WH-rGO)based on reduced graphene oxide(rGO)nanosheets and WO_(3)(rGO-WO_(3))seed layer via a hydrothermal *** incorporation of rGO not only promotes the uniform growth of hydrated WO_(3) film,enhancing ion transport but also introduces oxygen vacancies,creating an efficient conduction pathway for charge *** resulting WH-rGO film exhibits impressive performance,achieving 71% optical modulation at 700 nm,with bleaching and coloring times of 4.2 and 1.0 *** coloration efficiency is calculated at 156.11 cm^(2)·C^(-1),and the optical modulation is maintained at 93% of the initial optical modulation after 1000 cycles applied in the +1.0 and -1.1 V potential *** work offers new insights into the role of oxygen vacancies in enhancing the electrochromic properties of hydrated WO_(3) films through the addition of *** also provides a promising approach for the synthesis of electrochromic materials,facilitating their application in smart window technologies.

关键词： electrochromic film hydrated tungsten oxide reduced graphene oxide oxygen vacancy

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Reshaping Electrolyte Solvation Structure for High-Energy Aqueous Batteries

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Energy & Environmental materials 2022年第3期5卷 686-687页

作者： Shuailei Liu Jinping Liu School of Chemistry Chemical Engineering and Life ScienceState Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan 430070China

A highlight on reshaping aqueous electrolyte solvation structure for highenergy batteries is ***,the recent key design routes for regulating solvation structure to widen electrochemical stability window(ESW)of aqueous electrolyte are briefly ***,the groundbreaking work of Wang et *** reshaping electrolyte structure using urea as the diluent is ***,the significance of Wang's work is highlighted.

关键词： aqueous electrolyte structure CO(NH_2)_2 electrochemical stability window energy density

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A review on additive manufacturing of ceramic matrix composites

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Journal of materials Science & technology 2023年第7期138卷 1-16页

作者： Jinxing Sun Daorong Ye Ji Zou Xiaoteng Chen Yue Wang Jinsi Yuan Haowen Liang Hongqiao Qu Jon Binner Jiaming Bai Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055China School of Metallurgy and Materials University of BirminghamB152TTUK State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Additive manufacturing(AM)of ceramic matrix composites(CMCs)has enabled the production of highly customized,geometrically complex and functionalized parts with significantly improved properties and functionality,compared to single-phase ceramic *** also opens up a new way to shape damage-tolerant ceramic composites with co-continuous phase reinforcement inspired by natural ***,a large variety of AM techniques has been successfully applied to fabricate CMCs,but variable properties have been obtained so *** article provides a comprehensive review on the AM of ceramic matrix composites through a systematic evaluation of the capabilities and limitations of each AM technique,with an emphasis on reported results regarding the properties and potentials of AM man-ufactured ceramic matrix composites.

关键词： Additive manufacturing Ceramic matrix composites 3D printing Mechanical properties Bioinspired composites

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Transformation of Undesired Li_(2)CO_(3)into Lithiophilic Layer Via Double Replacement Reaction for Garnet Electrolyte Engineering

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Energy & Environmental materials 2022年第3期5卷 962-968页

作者： Jiaxu Zhang Ruohan Yu Jun Li Huiyu Zhai Gangjian Tan Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China International School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

Garnet-type solid-state electrolytes(SSEs)are a remarkable Li-ion electrolyte for the realization of next-generation all-solid-state lithium batteries due to their excellent stability against Li metal as well as high ionic conductivities at room ***,garnet electrolytes always contain undesired and hardly removable Li_(2)CO_(3) contaminations that have persistently large resistance and unstable interface contact with Li *** is a critical bottleneck for the practical application of garnet ***,we design a novel strategy to completely root out Li_(2)CO_(3) both inside and on the surface of *** is achieved by a so-called double replacement reaction between Li_(2)CO_(3) and SiO_(2) during one-step hot press process for garnet electrolyte *** leads to in-situ transformation of LixSiOy(LSO)mostly locating around the grain boundaries of *** to the higher ion conductivity and better electrochemistry stability of LSO than Li_(2)CO_(3),the modified garnet electrolyte shows much improved electrochemical ***,the wettability between modified garnet electrolyte and lithium metals was significantly enhanced in the absence of surface Li_(2)CO_(3).As a proof of concept,an assembled Li symmetric cell with modified garnet electrolyte displays a high critical current density(CCD)of 0.7 mA cm^(-2)and a low interfacial impedance(5Ωcm^(2))at 25℃.These results indicate that the upcycling of Li_(2)CO_(3)is a promising strategy to well-address the degradation and interfacial issue associated with garnet electrolytes.

关键词： double replacement reaction garnet electrolytes lithiophilic layer solid-state lithium batteries

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Polydopamine-assisted in-situ formation of dense MOF layer on polyolefin separator for synergistic enhancement of lithium-sulfur battery

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Nano Research 2022年第9期15卷 8048-8055页

作者： Xiuxiu Wu Cheng Zhou Chenxu Dong Chunli Shen Binbin Shuai Cheng Li Yan Li Qinyou An Xu Xu Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China International School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

The separator is of great significance to alleviate the shuttle effect and dendrite growth of lithium-sulfur ***,most of the current commercial separators cannot meet these requirements *** this work,a dense metal-organic-framework(MOF)modification layer is in-situ prepared by the assistant of polydopamine on the polypropylene *** to the unique structure and synergistic effect of polydopamine(PDA)and zeolitic imidazolate framework-8(ZIF-8),the functional separator can not only trap the polysulfides effectively but also promote the transport of lithium *** a result,the battery assembled with the functional separator exhibits excellent cycle *** capacity remains 711 mAh·g^(−1)after 500 cycles at 2 C,and the capacity decay rate is as low as 0.013%per *** symmetrical battery is cycled for 1,000 h at 2 mA·cm^(−2)(2 mAh·cm^(−2))with the plating/stripping overpotential of 20 *** the same time,the modification separator shows a higher lithium ion transference number(0.88),better thermal stability and electrolyte wettability than the unmodified separator.

关键词： metal-organic frameworks in-situ growth polysulfides shuttle effect gradient distribution

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Constructing electron-blocking grain boundaries in garnet to suppress lithium dendrite growth

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Journal of advanced Ceramics 2024年第2期13卷 166-175页

作者： Xing Xiang Zecheng Fang Congkun Du Zhenzhen Zhao Jiajia Chen Yanhua Zhang Huihu Wang Chenhuinan Wei Fei Chen Qiang Shen Hubei Provincial Key Laboratory of Green Materials for Light Industry Hubei University of TechnologyWuhan 430068China Hubei Longzhong Laboratory Wuhan University of Technology Xiangyang Demonstration ZoneXiangyang 441000China Collaborative Innovation Center of Green Light-weight Materials and Processing Hubei University of TechnologyWuhan 430068China New Materials and Green Manufacturing Talent Introduction and Innovation Demonstration Base Hubei University of TechnologyWuhan 430068China State Key Lab of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is considered as a promising solid-state electrolyte due to its high ionic conductivity,wide electrochemical window,and excellent electrochemical ***,its application in solid-state lithium metal batteries(SSLMBs)is impeded by the growth of lithium dendrites in LLZO due to some reasons such as its high electronic *** this study,lithium fluoride(LiF)was introduced into Ta-doped LLZO(LLZTO)to modify its grain boundaries to enhance the performance of SSLMBs.A nanoscale LiF layer was uniformly coated on the LLZTO grains,creating a threedimensional continuous electron-blocking network at the grain *** from the electronic insulator LiF and the special structure of the modified LLZTO,the symmetric cells based on LLZO achieved a high critical current density(CCD)of 1.1 mA·cm^(-2)(in capacity-constant mode)and maintained stability over 2000 h at 0.3 mA·cm^(-2).Moreover,the full cells combined with a LiFePO_(4)(LFP)cathode,demonstrated excellent cycling performance,retaining 97.1% of capacity retention after 500 cycles at 0.5 ***,this work provides a facile and effective approach for preparing a modified electrolyte suitable for high-performance SSLMBs.

关键词： solid electrolyte garnet lithium dendrite microstructure solid-state batteries

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Probing the Nucleation and Growth Kinetics of Bismuth Nanoparticles via In-situ Transmission Electron Microscopy

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Journal of Wuhan University of technology(materials Science) 2024年第4期39卷 877-887页

作者：王浪李超凡 RAN Maojin YUAN Manman 胡执一 LI Yu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Nanostructure Research Centre(NRC) Wuhan University of TechnologyWuhan 430070China Institute of Chemistry Henan Academy of SciencesZhengzhou 450002China Henan Academy of Sciences Zhengzhou 450046China

The nucleation and growth mechanism of nanoparticles is an important theory,which can guide the preparation of ***,it is still lacking in direct observation on the details of the evolution of intermediate state structure during nucleation and *** this work,the evolution process of bismuth nanoparticles induced by electron beam was revealed by in-situ transmission electron microscopy(TEM)at atomic *** experimental results demonstrate that the size,stable surface and crystallographic defect have important influences on the growth of Bi *** non-classical growth paths including single crystal growth and polycrystalline combined growth,as well as,corresponding layer-by-layer growth mechanism along{012}stable crystal plane of Bi nanoparticles with dodecahedron structure were revealed by in-situ TEM *** results provide important guidance and a new approach for in-depth understanding of the nucleation and growth kinetics of nanoparticles.

关键词： bismuth nanoparticles crystal growth transmission electron microscopy in-situ electron microscopy

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