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The pathway toward practical application of lithium-metal anodes for non-aqueous secondary batteries

National Science Review 2022年第8期9卷 194-210页

作者： Panlong Li Zhong Fang Xiaoli Dong Congxiao Wang Yongyao Xia Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Institute of New Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Fudan University

The revolution of automotive vehicles(from petrol vehicles to electric vehicles) has set high demands for the performance of batteries. lithium-metal batteries(LMBs) show great potential owing to their high energy density but encounter poor cycle life and safety issues. It is of great significance to reveal LMB failure mechanisms and understand their relationship with battery performance. This review presents an overview of the state-of-the-art Li-metal anodes, with an emphasis on two typical failure modes: capacity degradation and dendritic growth of Li metal. The critical correlations between the composition, structure and failure are explained point by point. The chemical and electrochemical stabilities of the lithium anode are discussed.Particularly, for the first time, five types of lithium-metal anodes are classified to develop a comprehensive understanding of LMBs. Furthermore, strategies are suggested to improve the practical performance of LMBs, including material innovation, electrolyte modification and advanced characterization.

关键词： lithium-metal anode failure mode concentration polarization dead Li

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Stabilizing the Electrochemistry of lithium-Selenium Battery via In situ Gelated Polymer Electrolyte: A Look from anode

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Chemical Research in Chinese Universities 2021年第2期37卷 298-303页

作者： WANG Wen-Peng ZHANG Juan LI Xue-Ting YIN Ya-Xia XIN Sen GUO Yu-Guo 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)Beijing100190P.R.China University of Chinese Academy of Sciences(UCAS) Beijing100049P.R.China

Li metal possesses a high theoretical specific capacity,high electronic conductivity,and a low electrochemical potential,making it a promising anode material for building next-generation rechargeable metal batteries.In case conventional liquid electrolytes were used,and the anode using Li metal has been hindered by unstable(electro)chemistry at Li/electrolyte interface and the accompanied dendrite issue.Specifically,for the Li-Se batteries,the dissolution and shuttle of polyselenide intermediates lead to the deposition of poorly-conductive species on the anode,which further aggravates the chemical environment at the anode.In this work,we proposed to stabilize the Li-Se electrochemistry by constructing a gel polymer electrolyte via in situ gelations of conventional ether-based electrolytes at room temperature.The results demonstrate that the in situ gelated electrolyte helps to build electrochemically stable electrode/electrolyte interfaces and promote the efficient transfer of charge carriers across the interface.Compared with the liquid electrolytes,the gelated electrolyte shows improved chemical compatibility with the Li metal anode,which effectively alleviates the unfavorable side reactions and dendrite formation at the anode/electrolyte interface,and the polyselenide shuttle from the cathode to the anode.As a result,the Li-Se battery shows a higher Coulombic efficiency and improved cycling performance.

关键词： lithium-metal anode Gel polymer electrolyte In situ polymerization lithium-selenium battery

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A Review of Solid Electrolyte Interphase(SEI)and Dendrite Formation in lithium Batteries

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Electrochemical Energy Reviews 2023年第1期6卷 680-725页

作者： Borong Li Yu Chao Mengchao Li Yuanbin Xiao Rui Li Kang Yang Xiancai Cui Gui Xu Lingyun Li Chengkai Yang Yan Yu David P.Wilkinson Jiujun Zhang College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina Key Laboratory of Eco-Materials Advanced Technology(Fuzhou University) Fuzhou UniversityFuzhou 350108FujianChina Department of Chemical and Biochemical Engineering University of British ColumbiaVancouverBC V6T1W5Canada Institute for Sustainable Energy/College of Sciences Shanghai UniversityShanghai 200444China

lithium-metal batteries with high energy/power densities have significant applications in electronics,electric vehicles,and stationary power plants.However,the unstable lithium-metal-anode/electrolyte interface has induced insufficient cycle life and safety issues.To improve the cycle life and safety,understanding the formation of the solid electrolyte interphase(SEI)and growth of lithium dendrites near the anode/electrolyte interface,regulating the electrodeposition/electrostripping processes of Li^(+),and developing multiple approaches for protecting the lithium-metal surface and SEI layer are crucial and necessary.This paper comprehensively reviews the research progress in SEI and lithium dendrite growth in terms of their classical electrochemical lithium plating/stripping processes,interface interaction/nucleation processes,anode geometric evolution,fundamental electrolyte reduction mechanisms,and effects on battery performance.Some important aspects,such as charge transfer,the local current distribution,solvation,desolvation,ion diffusion through the interface,inhibition of dendrites by the SEI,additives,models for dendrite formation,heterogeneous nucleation,asymmetric processes during stripping/plating,the host matrix,and in situ nucleation characterization,are also analyzed based on experimental observations and theoretical calculations.Several technical challenges in improving SEI properties and reducing lithium dendrite growth are analyzed.Furthermore,possible future research directions for overcoming the challenges are also proposed to facilitate further research and development toward practical applications.

关键词： lithium-metal anode Solid electrolyte interphase(SEI) Dendrite formation lithium batteries Classical electrochemical processes Additives Heterogeneous nucleation Asymmetric processes Solvation structure Desolvation In situ characterization of nucleation

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lithium deposition behavior in hard carbon hosts:Optical microscopy and scanning electron microscopy study

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Nano Research 2023年第6期16卷 8368-8376页

作者： Ge Zhou Yulin Zhao Chuan Hu Zhenzhen Ren Hong Li Liping Wang School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731China Tianmu Lake Institute of Advanced Energy Storage Technologies Changzhou 213300China Key Laboratory for Renewable Energy Institute of PhysicsChinese Academy of SciencesBeijing 100190China

lithium(Li)metal is an ideal anode for the next generation high-energy-density batteries.However,it suffers from dendrite growth,side reactions,and infinite relative volume change.Effective strategies are using porous carbons or surface modification carbons to guide Li deposition into their pores.While the Li deposition behavior is still ambiguous.Here,we systematically determine their deposition behavior in various surface-modified carbons and in different electrolytes via optical microscopy and scanning electron microscopy study.It is found that Li will not spontaneously deposit into the carbon pores,which is significantly dependent on the carbon surface,current density,areal capacity,and electrolyte.Thus,a“lithiophilic”modified commercial hard carbon with Ag is developed as a stable“host”and efficient surface protection derived from the localized high-concentration electrolyte exhibits a pretty low volume change(5.3%)during cycling at a current density of 2 mA·cm^(−2)and an areal capacity of 2 mAh·cm^(−2).This strategy addresses the volume change and dendrite problems by rationally designed host and electrolyte,providing a broad perspective for realizing Li-metal anode.

关键词： lithium-metal anode lithium deposition behavior hard carbon host lithiophilic sites localized high-concentration electrolyte

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In situ formed cross-linked polymer networks as dual-functional layers for high-stable lithium metal batteries

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Journal of Energy Chemistry 2023年第4期79卷 253-262页

作者： Lei Shi Wanhui Wang Chunjuan Wang Yang Zhou Yuezhan Feng Tiekun Jia Fang Wang Zhiyu Min Ji Hu Zhigang Xue School of Materials Science and Engineering School of Environmental Engineering and ChemistryLuoyang Institute of Science and TechnologyLuoyang 471023HenanChina Key Laboratory for Material Chemistry of Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina Key Laboratory of Advanced Materials Processing&Mold(Ministry of Education) National Engineering Research Center for Advanced Polymer Processing TechnologyZhengzhou UniversityZhengzhou 450002HenanChina Henan Intelligent Manufacturing Engineering Technology Research Center for Building Profile Luoyang Institute of Science and TechnologyLuoyang 471023HenanChina Henan Province International Joint Laboratory of Materials for Solar Energy Conversion and lithium Sodium based Battery Luoyang Institute of Science and TechnologyLuoyang 471023HenanChina

lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to industry.Herein,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV irradiation.Owing to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in advance.The intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.

关键词： lithium-metal anode Humid-resistant protective film Solid-state polymer electrolytes Cross-linked polymers

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Sustained‑Release Nanocapsules Enable Long‑Lasting Stabilization of Li anode for Practical Li‑metal Batteries

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Nano-Micro Letters 2020年第12期12卷 239-250页

作者： Qianqian Liu Yifei Xu Jianghao Wang Bo Zhao Zijian Li Hao Bin Wu School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027People’s Republic of China

A robust solid-electrolyte interphase(SEI)enabled by electrolyte additive is a promising approach to stabilize Li anode and improve Li cycling efficiency.However,the self-sacrificial nature of SEI forming additives limits their capability to stabilize Li anode for long-term cycling.Herein,we demonstrate nanocapsules made from metal–organic frameworks for sustained release of LiNO3 as surface passivation additive in commercial carbonate-based electrolyte.The nanocapsules can offer over 10 times more LiNO3 than the solubility of LiNO3.Continuous supply of LiNO3 by nanocapsules forms a nitride-rich SEI layer on Li anode and persistently remedies SEI during prolonged cycling.As a result,lifespan of thin Li anode in 50μm,which experiences drastic volume change and repeated SEI formation during cycling,has been notably improved.By pairing with an industry-level thick LiCoO2 cathode,practical Li-metal full cell demonstrates a remarkable capacity retention of 90%after 240 cycles,in contrast to fast capacity drop after 60 cycles in LiNO3 saturated electrolyte.

关键词： metal–organic frameworks LiNO3 Nanocapsules lithium-metal anode lithium-metal batteries

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