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lithium film with abundant stepped structures: A promising route for homogeneous Li ion deposition to conquer lithium dendrite issue and its action mechanism

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Journal of Energy Chemistry 2022年第9期31卷 166-175,I0006页

作者： Yong Zhang Shu-Qin Song Yong Gao Tian-Fu Liu Hong Zhao Department of Materials Science and Engineering Dalian Jiaotong UniversityDalian 116028LiaoningChina The Key Lab of Low-carbon Chemistry&Energy Conservation of Guangdong Province PCFM LabSchool of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou510275GuangdongChina Institute of Science and Technology for New Energy Xi'an Technological UniversityXian 710021ShaanxiChina Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023LiaoningChina

lithium is considered to be the ‘‘holy grail” for the application of energy storage due to its highest theoretical capacity and lowest anode potential. However, one of the grand difficulties in the development of lithium-based batteries is the lithium dendrite growth that leads to capacity fading and electrode degradation over long-term cycling. Compared with conventional electrolyte modifications, artificial solid electrolyte interfaces(SEI) synthesis and framework designing approaches, tuning surface morphology of lithium anode is the direct route to induce homogeneous Li ion deposition. Due to the high chemical activity of lithium metal, however, controllable growth of lithium micro/nanostructures by traditionally chemical approaches is still a big challenge. Herein, we have developed a facile compression route to fabricate lithium anode with abundant stepped lithium structures. The electrochemical results demonstrate that the dendritic growth issue is effectively suppressed by orderly arranged stepped lithium structures. After 90 cycles, a high discharge capacity of 954 mAh g^(-1) is achieved, which is 2.7times that of the uncompressed lithium anode(342 mAh g). First-principles calculations reveal that the orderly arranged stepped lithium structures are lithiophilic active sites to adsorb Li ion, which contributes to homogeneous deposition of Li ion on lithium anode, eventually solving the lithium dendrite issue. This work paves a new road to suppress dendritic growth, which will provide some new ideas to design long recycling sodium, potassium and zinc, and other metal anode batteries.

关键词： lithium dendrite Steps/edges Active sites Compression

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A composite PEO electrolyte with amide-based polymer matrix for suppressing lithium dendrite growth in all-solid-state lithium battery

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Chinese Chemical Letters 2022年第8期33卷 3894-3898页

作者： Menghan Ge Xiaoyu Zhou Yinping Qin Yang Liu Jingjing Zhou Xiaolei Wang Bingkun Guo Materials Genome Institute Shanghai UniversityShanghai 200444China Department of Chemical and Materials Engineering University of AlbertaEdmontonAlberta T6G 2R3Canada

The lithium dendrite growth is still a serious challenge and impeding the realistic applications of all-solid-state lithium batteries.In view of the amide containing sediment layer can be stable on lithium/cathodes,a composite polymer electrolyte with amide-based matrix is in-situ built on porous electrodes.With the introduction of amide,the polymer electrolyte presents excellent ability to inhibit lithium dendrite growth and makes the Li/Li symmetric battery stably work for 500 h with a good ionic conductivity of 4.25×10^(-5)S/cm at 40℃.The solid electrolyte also shows a wide electrochemical stable window and good interface contact with the porous cathode.Utilizing this composite polymer electrolyte,the all-solid-state Li/LiFePO_(4) battery shows an initial discharge capacity of 146.5 mA h/g at 0.1 C under 40℃ and remains 81.4%in 100 cycles.The polymer electrolyte also can present better properties after modification.These results demonstrate that the presented PA-based composite polymer electrolyte could be served as a good electrolyte candidate for all-solid-state lithium-ion batteries.

关键词： Composite Amide lithium dendrite Solid state electrolyte Li metal battery

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Bifunctional separator with high thermal stability and lithium dendrite inhibition toward high safety lithium-ion batteries

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Chinese Chemical Letters 2023年第5期34卷 553-556页

作者： Miaomiao Su Yifu Chen Suqing Wang Haihui Wang School of Chemistry&Chemical Engineering South China University of TechnologyGuangzhou 510640China School of Chemical Engineering Tsinghua UniversityBeijing 100084China

Coating inorganic ceramic particles on commercial polyolefin separators has been considered as an effective strategy to improve thermostability of separator.However,the introduction of the coating layer could induce pore blockage on the surface of the polyolefin separator.Herein,a ceramic composite layer that consists of alumina nanoparticles(n-Al_(2)O_(3))and halloysite nanotubes(HNTs)is designed to modify the polyethylene(PE)separator(the modified separator is denoted as AH-PE).The HNTs with hollow nanotubular structure construct a light skeleton and provide fast ion transport channels while Al_(2)O_(3)particles function as heat-resistant fillers to inhibit the shrinkage of the separator at elevated temperatures.The total thickness of AH-PE separator is only 14μm.Consequently,the mass increment of AH-PE separator decreases from 5 g/m^(2)to 3.5 g/m^(2),and the Gurley value reduces by 23%,compared with Al_(2)O_(3)coated PE separator(A-PE).Due to the synergistic effects of Al_(2)O_(3)and HNTs,AH-PE separator exhibits highly improved thermal stability(almost no shrinkage at 170℃for 30 min),high Li^(+)transference number(up to 0.47),and long cycle life of 450 h for Li|Li cells.Moreover,the Li Fe PO_(4)/Li cells assembled with AH-PE separators demonstrate improved rate capability and safety performance.

关键词： Separator lithium dendrite Thermal stability Halloysite nanotubes lithium-ion batteries

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Recent progresses in the suppression method based on the growth mechanism of lithium dendrite

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Journal of Energy Chemistry 2018年第2期27卷 513-527页

作者： Xiaolong Xu Suijun Wang Hao Wang Chen Hu Yi Jin Jingbing Liu Hui Yan The College of Materials Science and Engineering Beijing University of Technology State Key Laboratory of Operation and Control of Renewable Energy & Storage Systems China Electric Power Research Institute

lithium secondary batteries（LSBs） with high energy densities need to be further developed for future applications in portable electronic devices, electric vehicles, hybrid electric vehicles and smart grids. lithium metal is the most promising electrode for next-generation rechargeable batteries. However, the formation of lithium dendrite on the anode surface leads to serious safety concerns and low coulombic efficiency.Recently, researchers have made great efforts and significant progresses to solve these problems. Here we review the growth mechanism and suppression method of lithium dendrite for LSBs’ anode protection. We also establish the relationship between the growth mechanism and suppression method. The research direction for building better LSBs is given by comparing the advantages and disadvantages of these methods based on the growth mechanism.

关键词： lithium dendrite Growth mechanism Suppression method lithium secondary battery

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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 stability.However,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 conductivity.In 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 boundaries.Benefiting 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 C.Therefore,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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PVdF-HFP-Based Gel Polymer Electrolyte with Semi-Interpenetrating Networks For dendrite-Free lithium Metal Battery

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Acta Metallurgica Sinica(English Letters) 2021年第3期34卷 417-424页

作者： Lu Liu Xiaodong Wang Chenhui Yang Peng Han Lei Zhang Li Gao Zirui Wu Bingxin Liu Ruiping Liu Department of Materials Science and Engineering China University of Mining and Technology(Beijing)Beijing 100083.China Department of Mechanical Engineering University of Alaska FairbanksFairbanksAK 99775-5905USA School of Mechanical Engineering Qinghai UniversityXining 810016China

The safety issues and lower energy density of the lithium metal batteries are the two main challenges that hinder their applications in the fields of electric vehicles and portable devices.In this work,the semi-interpenetrated polyvinylidene fluoride-hexafluoropropylene(PVdF-HFP)-based gel polymer electrolyte was synthesized through UV-curing method by employing the ethoxylated trimethylolpropane triacrylate(ETPTA)monomer.The semi-interpenetrating networks formed by polymerization of ETPTA and the high liquid absorption rate of the PVdF-HFP impart the as-prepared electrolyte with a high room temperature ionic conductivity of 3.17×10-3 s cm^(-1)and a high mechanical strength of 3.46 MPa.LiFePO4 was selected as cathode materials,and the active material loading of the cathode is about 4.2 mg cm-2.The electrolyte shows superior long-term cycling properties(127 mAh g^(-1)after 200 cycles at 0.5 C),excellent rate performance(113 mAh g^(-1)at1 C,80 mAh g^(-1)at 2 C,and the discharge capacity of 135 mAh g^(-1)can be restored when the rate goes back to 0.1 C)as well as good ability to inhibit the growth of lithium dendrite(about 150 h).The facile synthesis strategy and great electrochemical performance of the electrolyte make it a potential candidate for lithium metal batteries.

关键词： Gel polymer electrolyte PVdF-HFP UV-curing lithium dendrite

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Electrolyte additive maintains high performance for dendrite-free lithium metal anode

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Chinese Chemical Letters 2020年第5期31卷 1217-1220页

作者： Manshu Zhang Renjie Liua Zekun Wang Xiyuan Xing Yangai Liu Bingbing Deng Tao Yang Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes.National Laboratory of Mineral Materials School of Materials Science and Technology.China University of GeosciencesBeijing 100083China Shanxi Key Laboratory of Green Preparation and Functionalization for Inorganic Materials Xi'an Key Laboratory of Green Processing for Ceramic materialsSchool of Material Science and EngineeringShaanxi University of Science and TechnologyXi'an 710021China College of Materials&Environmental Engineering Hangzhou Dianzi University.Hangzhou 310036China

Because of their high capacity and low potential,lithium metal anodes are considered to be promising candidates for next generation electrode materials.However,the safety concerns and limited cycling life associated with uncontrollable dendrite growth hamper practical applications.In this work,the acidified cellulose ester,which is a mixed fiber microporous membrane film,was used as a novel electrolyte additive that effectively improves the cycle stability of the lithium metal anode and inhibits dendrite growth.The focus of this paper is on inhibiting the formation and growth of lithium dendrites.The coulombic efficiency of a Li|Cu battery with this acidified cellulose ester additive remains stable at 99%after 500 cycles under a current density of 1 mA/cm^2.Symmetric batteries also remain stable after 500 cycles(1000 h)under a current density of 1 mA/cm^2.These superior properties can be ascribed to the induced nucleation and the uniform distribution of lithium ion flux.This study uncovers an approach for effectively enabling stable cycling of dendrite-free lithium metal anodes.

关键词： lithium metal batteries Acidified cellulose ester lithium dendrite Electrolyte additive Stable cycling

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A functional gel polymer electrolyte based on PVDF-HFP/gelatin toward dendrite-free lithium metal batteries

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Nano Research 2024年第4期17卷 2790-2799页

作者： Xiaoyi Hu Kangli Liu Shijie Zhang Guosheng Shao S.Ravi P.Silva Peng Zhang State Center for International Cooperation on Designer Low-carbon and Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Zhengzhou Materials Genome Institute(ZMGI) ZhongyuanzhiguXingyang 450100China Nanoelectronics Center Advanced Technology InstituteUniversity of SurreyGuildfordGU27XHUK

The leakage of liquid electrolyte and the formation of lithium dendrites pose challenges to safety and stability of lithium metal batteries(LMBs).The appearance of gel polymer electrolyte(GPE)has obviously improved the safety of traditional LMBs.However,the limited inhibition of GPE on lithium dendrites is detrimental to the safety of LMBs.Herein,a kind of poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)/gelatin(GN)GPE with high ionic conductivity,high-temperature resistance,and flame-retardancy,was prepared by electrospinning and soaking method.Utilizing the electrospinning network of PVDF-HFP,its affinity to liquid electrolytes,makes this GPE more beneficial to ions transport and the formation of gel.And,the GN with sol–gel properties,enhances the mechanical property(13.5 MPa)of HFP-GN GPE.Meanwhile,X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)suggest that the attraction of polar groups of GN to Li+can regulate the distribution of Li+and protect Li anodes.Consequently,the application of HFP-GN GPEs to LMBs with cathodes of LiFePO_(4) and LiCoO_(2) deliver excellent electrochemical performances:after 300 cycles,the LiFePO_(4)/HFP-GN GPE/Li battery keeps a low capacity decay rate of 0.09%at 5 C;after 400 cycles at 2 C,the LiCoO_(2)/HFP-GN GPE/Li cell retains a high capacity retention of 74%.This GPE is demonstrated for the application prospect of safe LMBs.

关键词： poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP) gelatin polar groups lithium metal battery lithium dendrite

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Intrinsic lithiophilic carbon host derived from bacterial cellulose nanofiber for dendrite-free and long-life lithium metal anode

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Nano Research 2024年第5期17卷 4203-4210页

作者： Gangyi Xiong Jiayu Yu Yalan Xing Puheng Yang Shichao Zhang School of Materials Science and Engineering Beihang UniversityBeijing 100191China School of Physics Science and Nuclear Energy Engineering Beihang UniversityBeijing 100191China

Although lithium metal is considered a promising anode for advanced Li-S and Li-air batteries,the uncontrolled dendrite growth and infinite volume change impede its practical application.Herein,we report an ideal framework composed of carbonized bacterial cellulose(CBC)nanofibers,which shows intrinsic lithiophilicity to molten lithium without any lithiophilic surface modification.The wetting behavior of molten lithium can be significantly improved because its surface functional groups provide thermodynamical driving force,and the high surface roughness derived from nanocracks leads to rapid infusion in kinetics.The hybrid anode exhibits long cycle life up to 2000 h and excellent deep stripping-platting capacity up to 20 mAh·cm^(-2).When the anode is assembled with LiFePO_(4) cathode,the full cell delivers a good cycling stability up to 700 cycles.This is attributed to the intrinsic lithiophilic scaffold,which can not only lower the nucleation barrier of Li and provide uniform nucleation sites for stable Li stripping/plating,but also offer interspace to accommodate volume fluctuation of lithium during long cycling.This work provides a new manner to achieve a series of intrinsic lithiophilic carbon skeletons based on the large family of biomass materials and organic materials.

关键词： intrinsic lithiophilicity lithium metal anode bacterial cellulose lithium dendrite long cycling life

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Integrated interface configuration by in-situ interface chemistry enabling uniform lithium deposition in all-solid-state lithium metal batteries

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Journal of Energy Chemistry 2023年第5期80卷 458-465,I0011页

作者： Yu-Long Liao Jiang-Kui Hu Zhong-Heng Fu Chen-Zi Zhao Yang Lu Shuai Li Shi-Jie Yang Shuo Sun Xi-Long Wang Jia Liu Jia-Qi Huang Hong Yuan School of Materials Science&Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBejing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBejing 100084China Beijing Key Laboratory of Lignocellulosic Chemistry Beijing Forestry UniversityBeijing 100083China

All-solid-state lithium metal batteries(ASSLMBs)are considered as one of the ultimate goals for the development of energy storage systems due to their high energy density and high safety.However,the mismatching of interface transport kinetics as well as interfacial instability induces the growth of lithium dendrite and thus,leads to severe degradation of battery electrochemical performances.Herein,an integrated interface configuration(IIC)consisting of in-situ generated Li I interphase and Li-Ag alloy anode is proposed through in-situ interface chemistry.The IIC is capable of not only regulating charge transport kinetics but also synchronously stabilizing the lithium/electrolyte interface,thereby achieving uniform lithium platting.Therefore,Li||Li symmetric cells with IIC achieve a critical current density of up to 1.6 mA cm^(-2)and achieve stable cycling over 1600 hours at a high current density of 0.5 mA cm^(-2).Moreover,a high discharge capacity of 140.1 mA h g-1at 0.1 C is also obtained for the Li(Ni_(0.6)Co_(0.2)Mn_(0.2))O_(2)(NCM622)full battery with a capacity retention of 65.6%after 300 cycles.This work provides an effective method to synergistically regulate the interface transport kinetics and inhibit lithium dendrite growth for high-performance ASSLMBs.

关键词： All-solid-state lithium battery Sulfide solid electrolyte Interface chemistry lithium dendrite

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