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Novel single-ion conducting polymer electrolytes with high toughness and high resistance against lithium dendrites

Nano Research 2023年第6期16卷 8457-8468页

作者： David Fraile-Insagurbe Nicola Boaretto Itziar Aldalur Iñigo Raposo Francisco Javier Bonilla Michel Armand María Martínez-Ibañez Centre for Cooperative Research on Alternative Energies CIC energiGUNEBasque Research and Technology Alliance(BRTA)Alava Technology ParkAlbert Einstein 48Vitoria-Gasteiz 01510Spain University of the Basque Country(UPV/EHU) Barrio Sarrienas/nLeioa 48940Spain

Solid-state polymer electrolytes are considered as an alternative to classic liquid electrolytes,particularly for application in highenergy lithium metal batteries.With respect to common dual-ion conductors,single-ion conducting polymer electrolytes(SICPEs)are less affected by lithium dendrites growth and thus are particularly interesting for application in lithium metal batteries.In this work,novel SIC-PEs are developed,based on an ionomer having poly(ethylene-alt-maleimide)backbone and lithium phenylsulfonyl(trifluoromethanesulfonyl)imide pendant moieties,further blended with poly(ethylene oxide)(PEO)and poly(ethylene glycol)dimethyl ether(PEGDME).These SIC-PEs exhibit ionic conductivity around~7×10^(−6)S·cm^(−1) at 70℃,lithium transference number close to unity,and excellent mechanical properties,with fracture toughness over 30 J·cm^(−3).Additionally,the electrolytes show very high resistance against lithium dendrites growth,by cycling for more than 1200 h in Li°symmetric cells at a current density of 0.1 mA·cm^(−2).LiFePO4||Li°cells with these SIC-PEs were cycled at 70℃ and C/10,showing initial capacity of almost 160 mAh·g^(−1)and residual capacity of 45%after 100 cycles.This work shows that single-ion conducting polymer electrolytes based on poly(ethylene-alt-maleimide)backbone are promising materials for application as electrolytes or catholytes in lithium metal polymer batteries.

关键词： single-ion conductors solid-state Li metal batteries polymer electrolytes lithium dendrites transference number mechanical properties

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Inhibition of lithium dendrites and dead lithium by an ionic liquid additive toward safe and stable lithium metal anodes

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Chinese Chemical Letters 2022年第8期33卷 3951-3954页

作者： Shengjie Zhang Bin Cheng Yanxiong Fang Dai Dang Xin Shen Zhiqiang Li Ming Wu Yun Hong Quanbing Liu Guangzhou Key Laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources BiorefinerySchool of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006China Department of Chemical Engineering Beijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyTsinghua UniversityBeijing 100084China

The uncontrolled growth of lithium dendrites and accumulation of"dead lithium"upon cycling are among the main obstacles that hinder the widespread application of lithium metal anodes.Herein,an ionic liquid(IL)consisting of 1-methyl-1-propylpiperidinium cation(Pp_(13)^+) and bis(fluorosulfonyl)imide anion(FSI^(-)),was chosen as the additive in propylene carbonate(PC)-based liquid electrolytes to circumvent the shortcoming of lithium metal anodes.The optimal 1%Pp_(13) FSI acts as the role of electrostatic shielding,lithiophobic effect and participating in the formation of solid electrolyte interface(SEI)layer with enhanced properties.The in-situ optical microscopy records that the addition of IL can effectively inhibit the growth of lithium dendrites and the corrosion of lithium anode.This study delivers an effective modification to optimize electrolytes for stable lithium metal batteries.

关键词： Ionic liquid Piperidinium lithium metal anode Solid electrolyte interface lithium dendrites Dead lithium

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Touch Ablation of lithium dendrites via Liquid Metal for High-Rate and Long-Lived Batteries

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CCS Chemistry 2021年第1期3卷 686-695页

作者： Wenjie Wang Xiaohui Zhu Lei Fu College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072 The Institute for Advanced Studies(IAS) Wuhan UniversityWuhan 430072

High energy density lithium(Li)metal batteries have attracted great attention,but they are faced with challenges of cycling instability and safety hazards.Due to high activity and drastic volume changes of metallic Li,potential dendritic risks cannot be fully eliminated.Therefore,suppressing already existing Li dendrites must be evaluated.In addition,Li-active solids alloying with Li always face mechanical instability and fractures with cycling.Herein,we present touch ablation of dendrites by liquid metal,namely forming a defense layer on the electrode to directly react with the dendrites.Embrittlement,supercooling,and other liquid characteristics make the liquid gallium(Ga)exhibit continuous and reversible reactions with Li.The unique layout with a hierarchical porous structure inhibits upward growth of the dendrites.The protected Li||Li cells achieve stable cyclic performance even at 10 mA cm^(–2)and a large capacity of 5 mA h cm^(-2).

关键词： lithium metal batteries lithium dendrites liquid metal long-lived batteries protective layer

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Highly crystalline vinylene-linked covalent organic frameworks enhanced solid polycarbonate electrolyte for dendrite-free solid lithium metal batteries

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Nano Research 2022年第9期15卷 8083-8090页

作者： Kaige Zhang Chaoqun Niu Chengbing Yu Li Zhang Yuxi Xu School of Materials and Engineering Zhengzhou UniversityZhengzhou 450001China School of Engineering Westlake UniversityHangzhou 310024China School of Materials Science and Engineering Shanghai UniversityShanghai 201800China

The development of solid-state electrolytes(SSEs)with high ionic conductivity,outstanding electrochemical window,and promising mechanical strength is a key factor in realizing the commercialization of high energy density solid-state lithium metal batteries(LMBs).Covalent organic frameworks(COFs)are a functional crystalline material with highly customizable molecular networks and one-dimensional channel structures,thus showing great potential applications in SSEs.Herein,we design flexible COF-poly(vinyl ethylene carbonate)(PVEC)(abbreviated as COF-PVEC)composite electrolyte films with excellent ionic conductivity and high mechanical strength,enabling dendrite-free and long-term running solid-state LMBs.Owing to the lithiumphilic triazine and carbon–carbon double bonds groups in the COF skeleton,the obtained flexible COF-PVEC shows high ionic conductivity up to 1.11×10^(−4)S·cm^(−1)at 40℃,and enlarged electrochemical window up to 4.6 V(vs.Li^(+)/Li)compared with pure PVEC electrolyte.At the same time,the lithium dendrites are efficiently inhibited after discharge–charging cycles,due to the improved Young’s modulus(150 MPa)and ordered channels of COF.Using the various features of COF-PVEC,we assembled a solid-state full battery with LiFePO4 cathode,which showed superior rate capacity(151.8,146.2,139.2,128.1,113.7,and 100.8 mAh·g^(−1)at 0.1,0.2,0.5,1,1.5,and 2 C,respectively)and excellent long-term cycling stability(over 400 cycles at 1 C).We believe that the COF-based composite electrolyte can become one of the most promising high-performance SSEs for solid-state LMBs.

关键词： solid-state electrolytes covalent organic frameworks lithium dendrites solid-state lithium metal batteries

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Full-chain enhanced ion transport toward stable lithium metal anodes

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Journal of Energy Chemistry 2023年第4期79卷 390-397页

作者： Yuliang Gao Fahong Qiao Nan Li Jingyuan You Yong Yang Jun Wang Chao Shen Ting Jin Xi Li Keyu Xie State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi’an 710072ShaanxiChina School of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina Department of Applied Physics The Hong Kong Polytechnic UniversityHong Kong 999077China Shanghai Key Lab of Advanced High-temperature Materials and Precision Forming Shanghai Jiao Tong UniversityShanghai 200240China

The dendrite growth that results from the slow electrode process kinetics prevents the lithium(Li) metal anode from being used in practical applications. Here, full-chain enhanced ion transport for stabilizing Li metal anodes is proposed. Experimental and theoretical studies confirm that full-chain enhanced ion transport(electrocrystallization, mass transport in the electrolyte and diffusion in solid electrolyte interphase) under magnetoelectrochemistry contributes to a homogeneous, dense, and dendrite-free morphology. Specifically, the enhanced electrocrystallization behavior promotes the Li nucleation;the enhanced mass transport in the electrolyte alleviates the ion concentration gradient at the electrode surface, which helps to inhibit dendrite growth;and the enhanced diffusion in the solid electrolyte interphase further homogenizes the Li deposition behavior, obtaining regular and uniform Li particles.Consequently, the Li metal anode has exceptional cycling stability in both symmetric and full cells,and the pouch cell performs long cycles(170 cycles) in practice evaluation. This work advances fundamental knowledge of the magneto-dendrite effect and offers a new perspective on stabilizing metal anodes.

关键词： lithium metal anodes Ion transport Pouch cell lithium dendrites Magnetic field

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Dead lithium formation in lithium metal batteries:A phase field model

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Journal of Energy Chemistry 2022年第8期31卷 29-35,I0002页

作者： Rui Zhang Xin Shen Yu-Tong Zhang Xia-Lin Zhong Hao-Tian Ju Tian-Xiao Huang Xiang Chen Jun-Dong Zhang Jia-Qi Huang Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

lithium metal batteries are the most promising choices for next-generation high-energy–density batteries. However, there is little mechanism understanding on lithium dendrite growth during lithium plating and the dead lithium(the main component of inactive lithium) formation during lithium stripping. This work proposed a phase field model to describe the lithium stripping process with dead lithium formation.The coupling of galvanostatic conditions enables the phase field method to accurately match experimental results. The factors influencing the dead lithium formation on the increasing discharge polarization are revealed. Besides, the simulation of the battery polarization curve, the capacity loss peak, and the Coulomb efficiency is realized. This contribution affords an insightful understanding on dead lithium formation with phase field methods, which can contribute general principles on rational design of lithium metal batteries.

关键词： lithium metal batteries lithium metal anodes lithium dendrites Dead lithium lithium stripping Phase field methods Finite element methods

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Silicon-carbide fiber-reinforced polymer electrolyte for all-solid-state lithium-metal batteries

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Rare Metals 2022年第11期41卷 3774-3782页

作者： Wen-Qing Wei Bing-Qiang Liu Yan-Qing Wang Kai Yan Hao Zhang Yu-Song Qi School of Mechanical and Automation Weifang UniversityWeifang261061China Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo315201China College of Mechanical and Electronic Engineering Shandong University of Science and TechnologyQingdao266590China School of Mechanical and Electrical Weifang University of Science and TechnologyShouguang262700China

Silicon carbide(SiC) with various morphologies was employed as reinforcing fillers for poly(ethylene oxide)(PEO)-based solid polymer electrolytes(SPEs).Specific ally,the SiC nanoparticles with an average size of 5-10 μm endow a significant enhancement of the interaction between carbon atoms for the fillers and the oxygen atoms from the PEO-lithium bis(trifluoromethanesulfonyl)imide(LiTFSI) matrix,which provides rapid transport channels for mobile Li+and enhances the mechanical strength of SPEs.The SPEs reinforced with one-dimensional SiC nanoparticles exhibit superior Li^(+)conduction,good mechanical property,and uniform Li plating.Thus,a dendrite-free plating of lithium for 0.58 mAh at 0.1 mA·cm^(-2) and excellent cycle stability at various current densities for 250 h are achieved in Li/Li symmetric cells using SPEs electrolytes with 5.0 wt% SiC nanoparticles.Moreover,the LiFePO_(4)/Li full cells assembled using SPEs electrolytes with 5.0 wt% SiC nanoparticles provide a capacity of 151.5 mAh·g^(-1) at 0.1 mA·cm^(-2)(55℃),and maintained a Coulombic efficiency of 99% for 120 cycles.

关键词： All-solid-state batteries Polymer electrolyte Ionic conductivity Mechanical property lithium dendrites

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A flame retardant separator modified by MOFs-derived hybrid for safe and efficient Li-S batteries

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Journal of Energy Chemistry 2022年第1期31卷 372-384,I0010页

作者： Na Wu Junling Wang Can Liao Longfei Han Lei Song Yuan Hu Xiaowei Mu Yongchun Kan State Key Laboratory of Fire Science.CAS Key Laboratory of Soft Matter Chemistry University of Science and Technology of ChinaHefei 230026AnhuiChina Jiangsu Key Laboratory of Hazardous Chemicals Safety and Control College of Safety Science and EngineeringNanjing Tech UniversityNanjing 211816JiangsuChina

In this work,we have successfully prepared a novel separator modified with N,S co-doped carbon framework(named NSPCF)with confined CoS_(2) nanoparticles and rooted carbon nanotubes material(named NSPCF@CoS_(2))to apply for high-performance lithium-Sulfur batteries(Li-S batteries).Robust carbon structure with large specific surface can act as a physical barrier and possess physical adsorption effect on lithium polysulfides(LiPSs).In addition,highly-conductive carbon can improve integral conductivity,leading to the fast charge transport and reaction kinetics.Also,doping heteroatoms could form more active sites to adsorb LiPSs strongly so that modified separator could inhibit the shuttle effect effectively.Moreover,the presence of CoS_(2) further enhances the ability of modified separator to trap LiPSs owing to the Lewis acid-base action.As a result,the NSPCF@CoS_(2)@C-150 battery can deliver initial discharge capacities of 863.0,776.2,649.1 and 489.4 mAh g^(-1) at 0.1,0.5,1 and 2C with a high sulfur loading of 2.04 mg cm^(-2),respectively.Notably,when turning the current density back to 0.1 C,its discharge capacity can recover to 1008.7 mAh g^(-1).In addition,the modified separators exhibit outstanding capacities to restrain the growth of lithium dendrites.It is noteworthy that the flame retardant performances of Li-S batteries are improved dramatically owing to the novel structures of modified separators.This rationally designed separator endows Li-S batteries with higher safety and excellent electrochemical performances,providing a feasible strategy for practical application of Li-S batteries.

关键词： Metal-organic frameworks Shuttling behavior lithium dendrites Safety

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Elucidating the suppression of lithium dendrite growth with a void-reduced anti-perovskite solid-state electrolyte pellet for stable lithium metal anodes

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Journal of Energy Chemistry 2023年第2期77卷 62-69,I0003页

作者： Yu YeXinyan Ye Haoxian Zhu Juncao Bian Haibin Lin Jinlong Zhu Yusheng Zhao Shenzhen Key Laboratory of Solid State Batteries Southern University of Science and TechnologyShenzhen 518055GuangdongChina Academy for Advanced Interdisciplinary Studies&Department of Physics Southern University of Science and TechnologyShenzhen 518055GuangdongChina Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and TechnologyShenzhen 518055GuangdongChina Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices Southern University of Science and TechnologyShenzhen 518055GuangdongChina

Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery contender.Among the alternatives proposed as solid-state electrolyte,lithium-rich anti-perovskite(Li RAP)materials have drawn the most interest because of high theoretical Li^(+)conductivity,low cost and easy processing.Although solid-state electrolytes are believed to have the potential to physically inhibit the lithium dendrite growth,lithium-metal batteries still suffer from the lithium dendrite growth and thereafter the short circuiting.The voids in practical Li RAP pellets are considered as the root cause.Herein,we show that reducing the voids can effectively suppress the lithium dendrite growth.The voids in the pellet resulted in an irregular Li^(+)flux distribution and a poor interfacial contact with lithium metal anode;and hence the ununiform lithium dendrites.Consequently,the lithium-metal symmetric cell with void-reduced Li_(2)OHCl-HT pellet was able to display excellent cycling performance(750 h at 0.4 m A cm^(-2))and stability at high current density(0.8 m A cm^(-2)for 120 h).This study provides not only experimental evidence for the impact of the voids in Li RAP pellets on the lithium dendrite growth,but also a rational pellet fabrication approach to suppress the lithium dendrite growth.

关键词： Llithium-rich anti-perovskite Solid-state electrolytes Void-reduced pellets lithium dendrites lithium metal anodes

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The roles of MXenes in developing advanced lithium metal anodes

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Journal of Energy Chemistry 2022年第6期31卷 132-149,I0005页

作者： Nicolas Lucero Dayannara Vilcarino Dibakar Datta Meng-Qiang Zhao Department of Chemical and Materials Engineering Newark College of EngineeringNew Jersey Institute of TechnologyNewarkNJ 07103USA Jose Marti Stem Academy Union CityNJ 07087USA Department of Mechanical and Industrial Engineering Newark College of EngineeringNew Jersey Institute of TechnologyNewarkNJ 07103USA

lithium(Li) metal has emerged as the most promising anode for rechargeable Li batteries owing to its high theoretical specific capacities, low negative electrochemical potential, and superior electrical conductivity. Replacing the conventional graphite anodes with Li metal anodes(LMAs) provides great potential to exceed the theoretical limitations of current commercial Li-ion batteries, leading to nextgeneration high-energy–density rechargeable Li metal batteries(LMBs). However, further development of LMAs is hindered by several inherent issues, such as dangerous dendrite growth, infinite volume change, low Coulombic efficiency, and interfacial side reactions. MXenes, a family of two-dimensional(2 D) transition metal carbides and/or nitrides, have recently attracted much attention to address these issues due to their 2D structure, lithiophilic surface terminations, excellent electrical and ionic conductivity, and superior mechanical properties. Herein, an overview of recent advances in the roles of MXenes for stabilizing LMAs is presented. In particular, strategies of utilizing MXenes as the Li hosts, artificial protection layers, electrolyte additives, and for separator modifications to develop stable and dendrite-free LMAs are discussed. Moreover, a perspective on the current challenges and potential outlooks on MXenes for advanced LMAs is provided.

关键词： MXenes 2D materials lithium dendrites lithium metal anodes Stability

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