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Li-Ion Transport Mechanisms in Selenide-Based solid-state electrolytes in Lithium-Metal Batteries:A Study of Li_(8)SeN_(2),Li_(7)PSe_(6),and Li_(6)PSe_(5)X(X=Cl,Br,I)

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Energy & Environmental Materials 2024年第5期7卷 37-47页

作者： Wenshan Xiao Mingwei Wu Huan Wang Yan Zhao Qiu He International School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China College of Materials Science and Engineering Sichuan UniversityChengdu 610065China The Institute of Technological Sciences Wuhan UniversityWuhan 430072China

To achieve high-energy-density and safe lithium-metal batteries(LMBs),solid-state electrolytes(SSEs)that exhibit fast Li-ion conductivity and good stability against lithium metal are of great *** study presents a systematic exploration of selenide-based materials as potential SSE ***,Li_(8)SeN_(2)and Li_(7)PSe_(6)were selected from 25 ternary selenides based on their ability to form stable interfaces with lithium ***,their favorable electronic insulation and mechanical properties were ***,extensive theoretical investigations were conducted to elucidate the fundamental mechanisms underlying Li-ion migration in Li_(8)SeN_(2),Li_(7)PSe_(6),and derived Li_(6)PSe_(5)X(X=Cl,Br,I).Notably,the highly favorable Li-ion conduction mechanism of vacancy diffusion was identified in Li6PSe5Cl and Li_(7)PSe_(6),which exhibited remarkably low activation energies of 0.21 and 0.23 eV,and conductivity values of 3.85×10^(-2)and 2.47×10^(-2)S cm^(-1)at 300 K,*** contrast,Li-ion migration in Li_(8)SeN_(2)was found to occur via a substitution mechanism with a significant diffusion energy barrier,resulting in a high activation energy and low Li-ion conductivity of 0.54 eV and 3.6×10^(-6)S cm^(-1),*** this study,it was found that the ab initio molecular dynamics and nudged elastic band methods are complementary in revealing the Li-ion conduction *** both methods proved to be efficient,as relying on only one of them would be *** discoveries made and methodology presented in this work lay a solid foundation and provide valuable insights for future research on SSEs for LMBs.

关键词： Li-ion transport lithium argyrodites lithium-metal battery selenides solid-state electrolytes

Recent progress in solid-state electrolytes for alkali-ion batteries

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Science Bulletin 2017年第21期62卷 1473-1490页

作者： cheng jiang huiqiao li chengliang wang school of optical and electronic information huazhong university of science and technologywuhan 430074china school of materials science and engineering huazhong university of science and technologywuhan 430074china

solid-state electrolytes have a lot of advantages, including the inhibition of alkali metal dendrite growth,the elimination of liquid electrolyte leakage, the improvement of safety, the enhancement of energy density and power density, and the potential application in flexible electronics. Therefore, solid-state electrolytes have become one of the hottest topics in energy-storage research area. An up-to-date review on solid-state electrolytes is of not only scientific significance but also technological imperative. Here,recent progress in solid-state electrolytes for alkali ion batteries is summarized. Through this comprehensive review and the comparison of different solid-state electrolytes, we hope it can give a clear figure of the state-of-art status and the development trend of the future solid-state electrolytes.

关键词： solid-state electrolytes Lithium-ion batteries Sodium-ion batteries Energy storage

Covalent organic framework-based solid-state electrolytes for advanced batteries

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Science China Chemistry 2024年第12期67卷 4037-4062页

作者： Desheng Feng Zhen Qin Yumei Ren Yuxi Xu School of Materials Science and Engineering Zhengzhou University of AeronauticsZhengzhou 450046China School of Engineering Westlake UniversityHangzhou 310024China

The emergence of solid-state batteries(SSBs)has generated significant interest in the field of energy storage,primarily due to their advantages such as high safety,high energy density and long *** state electrolytes(SSEs)play a crucial role in SSBs,which not only affects the ion transport efficiency,but also relates to the overall performance and stability of the *** recent years,SSEs based on covalent organic frameworks(COFs)have become a research focus in the battery field because of their unique structural characteristics and excellent *** review aims to provide an overview of the application and latest progress of COF-based SSEs in the field of advanced ***,the structural features of COFs and their advantages as SSEs are briefly introduced,followed by a summary of the types of COF-based SSEs(including neutral COF-based SSEs and ionic COF-based SSEs).The latest research progress in lithium ion batteries(LIBs),lithium metal batteries(LMBs),proton exchange membrane fuel cells(PEMFCs)and other advanced batteries recently is also ***,we summarize and outlook the current research status,the challenges faced in practical application,the future research directions and application prospects of COF-based SSEs.

关键词： covalent organic framework solid-state electrolytes advanced batteries

A leap by the rise of solid-state electrolytes for Li-air batteries

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Green Energy & Environment 2023年第4期8卷 939-944页

作者： Kecheng Pan Minghui Li Weicheng Wang Shuochao Xing Yaying Dou Shasha Gao Zhang Zhang Zhen Zhou Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhou450001China Key Laboratory of Microelectronics and Energy of Henan Province Department of Physics and Electronic EngineeringXinyang Normal UniversityXinyang464000China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin300071China

Li-air batteries have attracted extensive attention because of their ultrahigh theoretical energy density. However, the potential safety hazard of flammable organic liquid electrolytes hinders their practical applications. Replacing liquid electrolytes with solidstate electrolytes(SSEs) is expected to fundamentally overcome the safety issues. In this work, we focus on the development and challenge of solid-state Li-air batteries(SSLABs). The rise of different types of SSEs, interfacial compatibility and verifiability in SSLABs are presented. The corresponding strategies and prospects of SSLABs are also proposed. In particular, combining machine learning method with experiment and in situ(or operando)techniques is imperative to accelerate the development of SSLABs.

关键词： solid-state Li-air batteries solid-state electrolytes Interfacial compatibility and verifiability

Polyimide covalent organic frameworks as efficient solid-state Li^(+) electrolytes

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Science China Chemistry 2024年第5期67卷 1647-1652页

作者： Xu Liu Shi Wang Siqi Liu Chengfang Liu Xiangchun Li Jian Wu Dazhi Li Shihao Xu Chongyang Liu Wen-Yong Lai state Key Laboratory of Organic Electronics and Information Displays(SKLOEID) Institute of Advanced Materials(IAM)School of Chemistry and Life SciencesNanjing University of Posts&TelecommunicationsNanjing 210023China

Covalent organic frameworks(COFs) are attractive porous crystalline materials with extremely high stability, easy functionalization, and open channels, which are expected to be unique ion conductors/transporters in lithium ion batteries(LIBs). Despite recent advances, low ion conductivity and low transference number, resulting in low charging/discharging rate, low energy density, and short battery life, are the main issues that limit their direct application as solid electrolytes in LIBs. Here, we designed and synthesized a novel polyimide COF, namely, TAPA-PDI-COF, with abundant C=O groups, which has been successfully employed as high-performance solid electrolytes by doping TAPA-PDI-COF and succinonitrile(SN). Both the well-defined nanochannels of COFs and SN confined in the well-aligned channels restricted the free migration of anions, while C=O on COFs and CN groups of SN enhanced Li^(+) transport, thus achieving a high ion conductivity of 0.102 m S cm^(-1)at 80 °C and a high lithium-ion transference number of 0.855 at room temperature. According to density functional theory(DFT)calculations, Li-ion migration mainly adopted in-plane transport rather than the axial pathway, which may be due to the shorter hopping distances in the planar pathway. The results suggest an effective strategy for the design and development of all-solidstate ionic conductors for achieving high-performance LIBs.

关键词： lithium ion batteries(LIBs) covalent organic frameworks(COFs) solid-state ion conductors solid-state electrolytes ion conductivity

Roles of metal element substitutions from the bimetallic solid state electrolytes in lithium batteries

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Particuology 2022年第6期20卷 51-71页

作者： Wen Yu Nanping Deng Lin Tang Kewei Cheng Bowen Cheng Weimin Kang state Key Laboratory of Separation Membranes and Membrane Processes National Center for International Joint Research on Separation MembranesTiangong UniversityTianjin 300387China School of Textile Science and Engineering Tiangong UniversityTianjin 300387China

All-solid-state lithium batteries(ASSLBs),receiving extensive attentions and studies,exhibit better safety,environmental friendliness,stability,wider electrochemical stability window and higher energy density than traditionally liquid lithium *** a variety of inorganic materials,with highly replaceable,the non-lithium metal elements emerge in endlessly and affect performances in diversiform *** to facile preparation,convertible structures and excellent properties,the lithium-containing bimetallic granular materials are often applied as important components of electrolytes in lithium *** this review,in terms of the properties of substituted elements,changing crystal structures,increasing vacancies or defects and improving the interfacial conductions,the roles of metal element substitutions of inorganic particles on the improvement of solid-state electrolytes are *** the applications of substituted strategies in ASSLBs as the host of inorganic particles electrolytes and as fillers or modifications for composite electrolytes are also investigated and *** also summarizes the current concerns and obstacles that need to be broken through,as well as provides a basis guide for the selection and optimization of inorganic particles.

关键词： Metal element substitutions Bimetallic inorganic particles solid-state electrolytes All-solid-state lithium batteries Mechanisms

Latest progresses and the application of various electrolytes in high-performance solid-state lithium-sulfur batteries

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Journal of Energy Chemistry 2023年第7期82卷 170-197,I0005页

作者： Yanan Li Nanping Deng Hao Wang Qiang Zeng Shengbin Luo Yongbing Jin Quanxiang Li Weimin Kang Bowen Cheng state Key Laboratory of Separation Membranes and Membrane Processes/National Center for International Joint Research on Separation Membranes Tiangong UniversityTianjin 300387China School of Textile Science and Engineering Tiangong UniversityTianjin 300387China Institute for Frontier Materials Deakin UniversityGeelong and Waurn PondsVictoria 3216Australia

With the emergence of some solid electrolytes(SSEs)with high ionic conductivity being comparable to liquid electrolytes,solid-state lithium-sulfur batteries(SSLSBs)have been widely regarded as one of the most promising candidates for the next generation of power generation energy storage batteries,and have been extensively *** many fundamental and technological issues still need to be resolved to develop commercially viable technologies,SSLSBs using SSEs are expected to address the present limitations and achieve high energy and power density while improving safety,which is very attractive to large-scale energy storage *** have been developed for many ***,there are few systematic discussions related to the working mechanism of action of various electrolytes in SSLSBs and the defects and the corresponding solutions of various *** fill this gap,it is very meaningful to review the recent progress of SSEs in *** this review,we comprehensively investigate and summarize the application of SSEs in LSBs to determine the differences which still exist between current progresses and real-world requirements,and comprehensively describe the mechanism of action of SSLSBs,including lithium-ion transport,interfacial contact,and catalytic conversion *** importantly,the selection of solid electrolyte materials and the novel design of structures are reviewed and the properties of various SSEs are ***,the prospects and possible future research directions of SSLSBs including designing high electronic/ionic conductivity for cathodes,optimizing electrolytes and developing novel electrolytes with excellent properties,improving electrode/-electrolyte interface stability and enhancing interfacial dynamics between electrolyte and anode,using more advanced test equipment and characterization techniques to analyze conduction mechanism of Li^(+)in SSEs are *** is hoped that this review can arouse people’s at

关键词： solid-state lithium sulfur batteries Working mechanism solid-state electrolytes Outstanding electrochemical performance Excellent safety

Ultrathin inorganic-organic solid-state electrolyte reinforced by a prefiberized LAGP continuous skeleton

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Science China Materials 2025年第1期68卷 199-206页

作者： Shiya Li Shuhao Wang Gaofeng Du Jianing Liang Zhaoming Tong Yanming Cui Jiu Lin Xiaoxiong Xu Xizheng Liu Tianyou Zhai Huiqiao Li state Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China Key Laboratory of Optoelectronic Chemical Materials and Devices(Ministry of Education) School of Optoelectronic Materials&TechnologyJianghan UniversityWuhan 430056China Zhejiang Funlithium New Energy Technology Co. Ltd.Ningbo 315201China

Inorganic-organic composite electrolyte is proved an effective way to enhance the overall performance of the ***,simply combining powder fillers with polymers is not sufficient for the application of composite *** this work,we designed an ultrathin organic-inorganic composite solid electrolyte with high mechanical strength and ionic conductivity,in which the inorganic Li1.5Al0.5Ge1.5(PO_(4))3(LAGP)solid electrolyte is prefiberized into a three-dimensional nanofiber network to serve as a self-supporting skeleton for the polyethylene oxide(PEO)*** continuous skeleton structure not only significantly improves the mechanical strength of the PEO-based electrolyte,but also forms a continuous lithium-ion conduction path,promoting the rapid migration of lithium *** fiber-reinforced composite electrolyte has an ionic conductivity of 8.27×10^(−4) S cm^(-1) at 60°C and a tensile strength of up to 4.29 ***,it exhibits a reduced overpotential and stable long-term cycling performance over 1700 h when used in Li/Li symmetric *** LiFePO_(4)(LFP)|Li cell assembled with the fiber-reinforced composite electrolyte also delivers a specific capacity of about 142 mAh g^(−1) over 300 cycles at 0.5 C and maintains good cycling *** work provides a novel idea for designing the next generation of safe and reliable organic-inorganic composite solid-state electrolyte membranes.

关键词： solid-state lithium metal batteries solid-state electrolytes polymer electrolytes LAGP structure design ultra-thin electrolyte membrane

Recent advances and future perspectives of Ruddlesden–Popper perovskite oxides electrolytes for all-solid-state batteries

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InfoMat 2024年第8期6卷 1-19页

作者： Chongyang Zhou Weibin Guo Jiayao Fan Naien Shi Yi Zhao Xu Yang Zhen Ding Min Han Wei Huang Strait Institute of Flexible Electronics(SIFE Future Technologies)Fujian Key Laboratory of Flexible ElectronicsFujian Normal University and Strait Laboratory of Flexible Electronics(SLoFE)Fuzhouthe People's Republic of China Jiangsu Key Laboratory of New Power Batteries And Jiangsu Key Laboratory of Biofunctional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjingthe People's Republic of China Institute of Advanced Materials(IAM) Nanjing University of Posts&TelecommunicationsNanjingthe People's Republic of China Frontiers Science for Flexible Electronics(FSCFE) MIIT Key Laboratory of Flexible Electronics(KloFE)Northwestern Polytechnical UniversityXi'anthe People's Republic of China

All-solid-state batteries equipped with solid-state electrolytes(SSEs)havegained significant interest due to their enhanced safety,energy density,andlongevity in comparison to traditional liquid organic electrolyte-based ***,many SSEs,such as sulfides and hydrides,are highly sensitiveto water,limiting their practical *** one class of important perovskites,theRuddlesden–Popper perovskite oxides(RPPOs),show great promise as SSEsdue to their exceptional stability,particularly in terms of water *** review,the crystal structure and synthesis methods of RPPOs SSEs are firstintroduced in ***,the mechanisms of ion transportation,including oxygen anions and lithium-ions,and the relevant strategies forenhancing their ionic conductivity are described in ***,theprogress made in developing flexible RPPOs SSEs,which are critical for flexibleand wearable electronic devices,has also been ***,thekey challenges and prospects for exploring and developing RPPOs SSEs in allsolid-state batteries are *** review presents in detail the synthesismethods,the ion transportation mechanism,and strategies to enhance theroom temperature ionic conductivity of RPPOs SSEs,providing valuableinsights on enhancing their ionic conductivity and thus for their practicalapplication in solid-state batteries.

关键词： all-solid-state batteries ionic conductivity improvement strategies Ruddlesden–Popper perovskite oxides solid-state electrolytes