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Electrolyte Design for Low‑Temperature li‑metal Batteries:Challenges and Prospects

Nano-Micro Letters 2024年第2期16卷 365-382页

作者： Siyu Sun Kehan Wang Zhanglian Hong Mingjia Zhi Kai Zhang Jijian Xu Department of Chemistry City University of Hong KongHong Kong 999077People’s Republic of China State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Haihe Laboratory of Sustainable Chemical TransformationsCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)College of ChemistryNankai UniversityTianjin 300071People’s Republic of China Department of Chemical and Biomolecular Engineering University of Maryland College ParkCollege ParkMD 20742USA

Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements in electrolyte chemistry need to be coupled with optimized electrode materials and tailored electrolyte/electrode interphases.Herein,this review critically outlines electrolytes’limiting factors,including reduced ionic conductivity,large de-solvation energy,sluggish charge transfer,and slow li-ion transportation across the electrolyte/electrode interphases,which affect the low-temperature performance of li-metal batteries.Detailed theoretical derivations that explain the explicit influence of temperature on battery performance are presented to deepen understanding.Emerging improvement strategies from the aspects of electrolyte design and electrolyte/electrode interphase engineering are summarized and rigorously compared.Perspectives on future research are proposed to guide the ongoing exploration for better low-temperature li-metal batteries.

关键词： Solid electrolyte interphase li metal Low temperature Electrolyte design Batteries

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The mechanism of external pressure suppressing dendrites growth in li metal batteries

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Journal of Energy Chemistry 2023年第4期79卷 489-494页

作者： Genming Lai Yunxing Zuo Junyu Jiao Chi Fang Qinghua liu Fan Zhang Yao Jiang liyuan Sheng Bo Xu Chuying Ouyang Jiaxin Zheng School of Advanced Materials Peking UniversityShenzhen Graduate SchoolShenzhen 518055GuangdongChina EACOMP Shenzhen 518055GuangdongChina Fujian Science&Technology Innovation Laboratory for Energy Devices of China(21C-LAB) Ningde 352100FujianChina PKU-HKUST ShenZhen-HongKong Institution Shenzhen 518055GuangdongChina

li metal is considered an ideal anode material for application in the next-generation secondary batteries.However,the commercial application of li metal batteries has not yet been achieved due to the safety concern caused by li dendrites growth.Despite the fact that many recent experimental studies found that external pressure suppresses the li dendrites growth,the mechanism of the external pressure effect on li dendrites remains poorly understood on the atomic scale.Herein,the large-scale molecular dynamics simulations of li dendrites growth under different external pressure were performed with a machine learning potential,which has the quantum-mechanical accuracy.The simulation results reveal that the external pressure promotes the process of li self-healing.With the increase of external pressure,the hole defects and li dendrites would gradually fuse and disappear.This work provides a new perspective for understanding the mechanism for the impact of external pressure on li dendrites.

关键词： li metal Machine learning potential Molecular dynamic simulation Dendrite External pressure

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Polymeric Wetting Matrix for a Stable Interface between Solid-state Electrolytes and li metal Anode

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Chinese Journal of Structural Chemistry 2022年第5期41卷 48-54页

作者： Haoran Song Shida Xue Shiming Chen Zijian Wang Yongli Song Jiawen li Zhibo Song Luyi Yang Feng Pan School of Advanced Materials Peking University Shenzhen Graduate SchoolShenzhen 518055China

Succinonitrile(SN)based solid-state electrolytes(SSEs)have potential applications in lithium(li)batteries due to their ease of preparation and high ionic conductivity at room temperature.Here,a novel SSE consisting of poly(vinylidene fluoride-hexafluoropropy-lene)(PVDF-HFP),poly(methyl methacrylate)(PMMA)and li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3) with SN is fabricated,where PMMA is added to serve as a polymer matrix for better wettability of SN.Due to the addition of PMMA,improved room-temperature ionic conductivity of the SSE is resulted.More importantly,better interfacial contact as well as more stable solid-state electrolyte(SEI)layer between SSE and li anode can be also obtained.As a result,homogeneous and dendrite-free li plating can be achieved for over 1000 h in li symmetric cells.When coupled with liNi_(0.5)Mn_(0.3)Co_(0.2)O_(2) cathode and li anode,the proposed SSE delivers excellent cycling stability and rate capability in full-cells.By implementing SSEs with a polymeric wetting agent,this work provides fresh perspectives on stabilizing the interface between SSEs and li metal anodes.

关键词： li metal li dendrite poly(methyl methacrylate) succinonitrile composite solid-state electrolyte

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Spatially controlled lithium deposition on li_(x)Cu_(y)P_(z) arrays enabling highly stable lithium metal batteries

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Journal of Materials Science & Technology 2023年第21期152卷 212-219页

作者： Ying Zhou Xiangru Sun Peiran Tan Yueming Wang Hongyang Dong Dejun li Tianjin International Joint Research Centre of Surface Technology for Energy Storage Materials College of Physics and Materials ScienceTianjin Normal UniversityTianjin 300387China

lithium(li)metal is a potential anode for high-energy-density batteries because of its low potential and ultrahigh capacity.Nevertheless,the li dendrites formation,the ununiform li deposition,and the growth of li dendrites hamper its application,especially under high deposition capacity/high rate.Here,a spatially controlled li deposition mode with array-oriented morphology is achieved based on the novel mixed ion/electron-conducting li_(x)Cu_(y)P_(z) arrays constructed on Cu foil,which can be facile fabricated via an in-situ transformation of metal phosphide.Theoretic calculations indicate the excellent lithiophilicity and low li diffusion barrier of the arrays,especially for the li_(2)CuP phase,which are conducive to ho-mogenizing the li nucleation/deposition of li.Moreover,such mixed conducting arrays promote fast li+diffusion via the continuous li+pathways as well as modulate the li+flux/electric field.Furthermore,the arrays with enlarged specific surface area and open spaces reduce the local current density and alle-viate the volume fluctuation of li.Consequently,a dendrite-free li anode is obtained under a high rate(20 mA cm^(–2))or a high deposition capacity(10 mAh cm^(–2)).In addition,even if the negative/positive ratio reduces to only 1.1,the full cells still perform outstanding stability for over 200 cycles.This work empha-sizes the importance of the design of the framework in terms of the intrinsic properties and structure and reveals a pathway for developing li metal batteries.

关键词： li metal li dendrites metal phosphates lithiophilic Mixed conductor Full cell

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Oxidization of fluid-like li metal with inherent lieli_(2)O interface from simulation insights

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Journal of Materiomics 2020年第4期6卷 692-701页

作者： Xia Lu Xingqun liao School of Materials Sun Yat-sen UniversityGuangzhou510275China Huizhou Highpower Technology Co.Ltd. Huizhou516000China

The oxidization of pure li is rarely discussed,but substantially important in the design and optimization,especially the failure mechanism of li metal anode for rechargeable batteries.In this context,the li metal and inherent lieli_(2)O interface after oxidization are examined using first principles calculations.The results demonstrated that in li itself,the li ion exhibits a fluid-like transport feature,especially in the vacancy-assisted migration.The fresh li surface can be oxidized quickly in air with a thick cover(mainly li oxides),and an inherent lieli_(2)O interface is,therefore,introduced.With the lowest surface energy,the li(111)plane is revealed with a strong capability of adsorbing O and N atoms to form the distorted Xli6(X=O,N,etc.)octahedra in the outmost surface layers.Although the li ion migrates fast in li itself,the lieli_(2)O interface shows a sluggish li diffusion kinetic in li_(2)O side.This ultimately leads to the li diffusion prefers to go along the interface boundary in li side,which loosens the lieli2O interface structure to result in the exfoliation of surface metastable li_(2)O spontaneously during electrochemical cycles in limetal batteries.

关键词： li metal li-li_(2)O interface Stability Kinetics li-metal batteries

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Polybenzimidazole functionalized electrolyte with li-wetting and self-fluorination functionalities for practical li metal batteries

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InfoMat 2022年第5期4卷 174-186页

作者： Dongjiang Chen Yuanpeng liu Chuan Xia Yupei Han Qingwei Sun Xuchang Wang Wei Chen Xian Jian Weiqiang Lv Jianyi Ma Weidong He National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and StructuresHarbin Institute of TechnologyHarbinChina School of Physics University of Electronic Science and Technology of ChinaChengduChina School of Materials and Energy University of Electronic Science and Technology of ChinaChengduChina Institute of Atomic and Molecular Physics Sichuan UniversityChengduSichuanChina

Rough li plating,low ionic conductivity,and low thermal stability of conventional electrolytes post-primary challenges for achieving reliable high-capacity rechargeable lithium batteries,for which lithiummetal is frequently proposed as themost promising anode material.Conventional low-polarity commercial polypropylene/polyethylene separators fail to support the application of high-energy-density li anodes due to their rigid physicochemical properties and the high reactivity of li metal,leading to fatal dendrite formation and vigorous exothermic reaction with electrolytes.Herein,we develop a li-wetting,flame-retardant binary polymer electrolyte by functionalizing poly(vinylidene fluoride)(PVDF)separators with nonflammable polybenzimidazole(PBI)to build safe room-temperature solid-state electrolyte membranes.A dendrite-free liFePO4 cell with the solid polymer electrolyte(SPE)delivers a discharge capacity of 127 mAh g^(-1) at 25℃ with a capacity retention of 87.5%after 500 cycles at 0.5℃(0.15 mA cm^(-2)).Phase-field simulations and density functional theory calculations demonstrate that the negatively charged benzimidazole chains of PBI own superior affinity to lithium bis(trifluoromethanesulfonyl)imide(liTFSI),and shares overlapping electron density with li anode,giving rise to accelerated li^(+)conduction at room temperature and uniform li electrodeposition at the electrolyte/li metal interface.The SPE is also flame-retardant since heat-resistant polytetrafluoroethylene and a dense,heat-blocking graphitized carbon layer are formed in intense heat throughdehydrogenation/fluorination of PVDF under the catalysis of Lewis base imidazole rings and the decomposition of benzimidazole rings in PBI.No such fire-resistant mechanism is ever reported in conventional electrolytes.

关键词： flame-retardant properties li metal polybenzimidazole solid polymer electrolyte uniform li deposition

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lithiophilic seeds and rigid arrays synergistic induced dendrite-free and stable li anode towards long-life lithium-oxygen batteries

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Journal of Energy Chemistry 2022年第10期31卷 268-276,I0006页

作者： Yue li Haichang Zhang Rui Zhang Junwei Sha liying Ma Dongdong Zhao Chunsheng Shi Naiqin Zhao School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin UniversityTianjin 300350China Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education Tianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072China China Science and Technology on Power Sources Laboratory Tianjin Institute of Power SourcesTianjin 300384China

High energy density lithium-oxygen battery(LOB) is currently regraded as a promising candidate for next-generation power system.However,the dendrite and instability issues of li metal anode lead to its poor cyclic stability and low energy density.In this work,lithiophilic Al_(2) O_(3) seeds induced rigid carbon nanotube arrays(CNTA)/three-dimensional graphene(3 DG) is developed as a host material for li anode,namely Al_(2) O_(3)-CNTA/3 DG.It is demonstrated that the lithiophilic feature of Al_(2) O_(3) seeds and the enhanced rigidity of arrays can synergistically induce the uniform li flux,inhibit the collapse of arrays,and stabilize electrolyte/electrode interfaces.As a result,the Al_(2) O_(3)-CNTA/3 DG-li anode delivers a high Coulombic efficiency above 97% after 140 cycles(8 mAh cm^(-2) at 4 mA cm^(-2)).With this anode and the breathable CNTA/3 DG cathode,the full LOB exhibits a significantly increased life-span up to 160 cycles(500 mAh g^(-1) at 100 mA g^(-1)),which is almost 3 times longer than that with pure li foil as the anodes.This work demonstrates a new approach to highly reversibly long-cycling performance of LOBs towards practical application.

关键词： Caron nanotube array Al_(2)O_(3) li-O_(2)battery li metal Anode

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In situ formed synaptic Zn@liZn host derived from ZnO nanofiber decorated Zn foam for dendrite-free lithium metal anode

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Nano Research 2023年第6期16卷 8345-8353页

作者： Jian Bao Hai-Juan Pei Xin-Yang Yue Xun-Lu li Cui Ma Rui-Jie Luo Chong-Yu Du Yong-Ning Zhou Department of Materials Science Fudan UniversityShanghai 200433China State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power-SourcesShanghai 200245China Department of Chemical Engineering Tsinghua UniversityBeijing 100084China

lithium metal is regarded as the most promising anode material for next generation high energy density lithium batteries due to its high theoretical capacity and lowest potential versus standard hydrogen electrode.However,lithium dendrite growth and huge volume change during cycling hinder its practical application.It is of great importance to design advanced li metal anodes to solve these problems.Herein,we report a ZnO-coated Zn foam as the host matrix to pre-store lithium through thermal infusing,achieving a Zn@ZnO foam supported li composite electrode(LZO).Needlelike ZnO nanofibers grown on the Zn foam greatly increase the surface area and enhance the lithiophilicity of the Zn foam.In situ formed synaptic liZn layer after lithium infusion can disperse local current density and lower li diffusion barrier effectively,leading to homogeneous li deposition behavior,thus suppressing dendrite formation.The porous Zn foam skeleton can accommodate volume variation of the electrode during longterm cycling.Benefiting from these merits,the LZO anode exhibits much better cycle stability and rate capability in both symmetrical and full cells with low voltage hysteresis than the bare li anode.This work opens a new opportunity in designing high performance composite li anode for lithium-metal batteries.

关键词： lithium batteries anode liZn alloy thermal infusion li metal

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A robust interphase via in-situ pre-reconfiguring lithium anode surface for long-term lithium-oxygen batteries

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Journal of Energy Chemistry 2022年第9期31卷 186-194,I0006页

作者： Pan Xu Xiaodong lin Zongqiang Sun Kaixuan li Wenjie Dou Qing Hou Zhiyou Zhou Jiawei Yan Mingsen Zheng Ruming Yuan Quanfeng Dong Collaborative Innovation Centre of Chemistry for Energy Materials(iChEM) State Key Laboratory of Physical Chemistry of Solid SurfacesDepartment of ChemistryCollege of Chemistry and Chemical EngineeringEngineering Research Centre of Electrochemical Technologies of Ministry of EducationXiamen UniversityXiamen 361005FujianChina

lithium-oxygen(li-O) battery is considered as one of the most promising alternatives because of its ultrahigh theoretical energy density. However, their cycling stability is severely restricted by the uncontrollable dendrite growth and serious oxygen corrosion issue on li surface. Herein, a sulfur-modified li surface can be successfully constructed via chemical reaction of guanylthiourea(GTU) molecule on li,which can induce the selectively fast decomposition of lithium bis(trifluoromethanesulfonyl)imide(liTFSI) to form a smooth and stable inorganics-rich solid-electrolyte interphase(IR-SEI) during the subsequent electrochemical process. Such an IR-SEI cannot only offer a highly reversible and stable li plating/stripping chemistry with dendrite-free property(10 mA cm^(-2)-10 mAh cm^(-2), > 0.5 years;3 mA cm^(-2)-3 m Ah cm^(-2), > 1 year) but also endows the li metal an anti-oxygen corrosion function, thereby significantly improving the cycling stability of li-Obatteries. This work provides a new idea for constructing functional solid-electrolyte interphase(SEI) to achieve highly stable li metal anode.

关键词： Solid-electrolyte interphase Guanylthiourea Sulfur-modified li surface li metal li-O_(2)batteries

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Tuning the electron transport behavior at li/LATP interface for enhanced cyclability of solid-state li batteries

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Nano Research 2023年第1期16卷 1634-1641页

作者： linshan Luo Feng Zheng Haowen Gao Chaofei Lan Zhefei Sun Wei Huang Xiang Han Ziqi Zhang Pengfei Su Peng Wang Shengshi Guo Guangyang lin Jianfang Xu Jianyuan Wang Jun li Cheng li Qiaobao Zhang Shunqing Wu Ming-Sheng Wang Songyan Chen Department of Physics Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient DevicesKey Laboratory of Low Dimensional Condensed Matter Physics(Department of Education of Fujian Province)Jiujiang Research InstituteXiamen UniversityXiamen 361005China State Key Lab of Physical Chemistry of Solid Surfaces College of MaterialsXiamen UniversityXiamen 361005China College of Materials Science and Engineering Nanjing Forestry UniversityNanjing 210037China Western Digital Corporation 951 Sandisk DrMilpitasCA 95035USA

An interlayer is usually employed to tackle the interfacial instability issue between solid electrolytes(SEs)and li metal caused by the side reaction.However,the failure mechanism of the ionic conductor interlayers,especially the influence from electron penetration,remains largely unknown.Herein,using li1.3Al0.3Ti1.7(PO4)3(LATP)as the model SE and liF as the interlayer,we use metal semiconductor contact barrier theory to reveal the failure origin of li/liF@LATP interface based on the calculation results of density functional theory(DFT),in which electrons can easily tunnel through the liF grain boundary with F vacancies due to its narrow barrier width against electron injection,followed by the reduction of LATP.Remarkably,an Al-liF bilayer between li/LATP is found to dramatically promote the interfacial stability,due to the highly increased barrier width and homogenized electric field at the interface.Consequently,the li symmetric cells with Al-liF bilayer can exhibit excellent cyclability of more than 2,000 h superior to that interlayered by liF monolayer(~860 h).Moreover,the li/Al-liF@LATP/liFePO4 solid-state batteries deliver a capacity retention of 83.2%after 350 cycles at 0.5 C.Our findings emphasize the importance of tuning the electron transport behavior by optimizing the potential barrier for the interface design in high-performance solid-state batteries.

关键词： solid-state electrolyte li metal liF Al electron transport interfacial barrier

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