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The Critical Role of Fillers in composite polymer electrolytes for Lithium Battery

Nano-Micro Letters 2023年第5期15卷 339-375页

作者： Xueying Yang Jiaxiang Liu Nanbiao Pei Zhiqiang Chen Ruiyang Li Lijun Fu Peng Zhang Jinbao Zhao College of Energy Xiamen UniversityXiamen 361102People’s Republic of China State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Centre of Chemistry for Energy MaterialsState-Province Joint Engineering Laboratory of Power Source Technology for New Energy VehicleEngineering Research Center of Electrochemical TechnologyMinistry of EducationCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China College of Energy Nanjing Technical UniversityNanjing 211816People’s Republic of China

With excellent energy densities and highly safe performance,solidstate lithium batteries(SSLBs)have been hailed as promising energy storage devices.Solid-state electrolyte is the core component of SSLBs and plays an essential role in the safety and electrochemical performance of the cells.composite polymer electrolytes(CPEs)are considered as one of the most promising candidates among all solid-state electrolytes due to their excellent comprehensive performance.In this review,we briefly introduce the components of CPEs,such as the polymer matrix and the species of fillers,as well as the integration of fillers in the polymers.In particular,we focus on the two major obstacles that affect the development of CPEs:the low ionic conductivity of the electrolyte and high interfacial impedance.We provide insight into the factors influencing ionic conductivity,in terms of macroscopic and microscopic aspects,including the aggregated structure of the polymer,ion migration rate and carrier concentration.In addition,we also discuss the electrode-electrolyte interface and summarize methods for improving this interface.It is expected that this review will provide feasible solutions for modifying CPEs through further understanding of the ion conduction mechanism in CPEs and for improving the compatibility of the electrode-electrolyte interface.

关键词： composite polymer electrolytes Fillers Ionic conductivity Electrode-electrolyte interface

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Ultrathin poly(cyclocarbonate-ether)-based composite electrolyte reinforced with high-strength functional skeleton

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Journal of Energy Chemistry 2023年第6期81卷 603-612,I0013页

作者： Xiaojiao Zheng Da Xu Ning Fu Zhenglong Yang Shanghai Key Laboratory of D&A for Metal-Functional Materials School of Materials Science and EngineeringTongji UniversityShanghai 200092China School of Chemical and Environmental Engineering Anyang Institute of TechnologyAnyang 455000HenanChina

composite polymer electrolytes(CPEs)are considered to be the most promising to break through the performance and safety limitations of traditional lithium-ion batteries because of their excellent electrochemical and mechanical properties.Aiming at the performance limitations of the most common polyether matrix such as poly(ethylene oxide)(PEO),a novel poly(cyclocarbonate-ether)polymer matrix was prepared by in-situ thermal curing,the weaker interaction between its C=O bond and Li^(+)can promote the rapid transport of Li^(+).Adding ionic liquid and active filler LLZTO to the matrix can synergistically reduce the crystallinity of matrix and promote the dissociation of lithium salts.In addition,a 3D functional skeleton made of polyacrylonitrile(PAN)and lithium fluoride(LiF)can greatly improve the mechanical strength of polymer matrix after cold pressing,and Li F is also conducive to interface stability.The thickness of the optimal sample(VP6L/CPL)was only 25μm,and its ionic conductivity,lithium ion transference number,and electrochemical stability window were as high as 7.17×10^(-4)S cm^(-1)(25℃),0.54 and 5.4 V,respectively,while the mechanical strength reaches 6.1 MPa,which can fully inhibit the growth of lithium dendrites.The excellent electrochemical performance and mechanical strength enable the assembled Li|VP6L/CPL|Li battery to be continuously charged for over 200 h and cycled stably for more than 2300 h,and Li|VP6L/CPL|LFP battery can be stably cycled for more than 400 and 550 cycles at 1 C(40℃)and 0.5 C(25℃),respectively.

关键词： composite polymer electrolytes polymer matrix 3D functional skeleton Plasticization Synergistic effect

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An artificial interphase enables stable PVDF-based solid-state Li metal batteries

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Nano Research 2024年第3期17卷 1482-1490页

作者： Mengjun Wu Jiangping Song Jiaheng Lei Haolin Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Chemistry School of ChemistryChemical Engineering and Life SciencesWuhan University of TechnologyWuhan 430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Foshan 528200China

composite polymer electrolytes(CPEs)have attracted much attention for high energy density solid-state lithium-metal batteries owing to their flexibility,low cost,and easy scale-up.However,the unstable Li/CPE interface is always challengeable for the practical utilization of CPEs.Herein,a polymer interlayer containing K+prepared by ultraviolet(UV)-curing precursor solution is coated on Li surface to stabilize the interface between poly(vinylidene difluoride)(PVDF)composite electrolytes and Li anode.Benefiting from the physical barrier of the interlayer,the continuous decomposition of PVDF is restrained and the intimate contact between electrode and electrolyte is also achieved to reduce the interface impedance.Moreover,the added K+is utilized to further regulate smooth Li deposition.As a consequence,the symmetric Li|Li cell with coated Li demonstrates steady cycling at 0.4 mAh·cm^(-2) and a high critical current density of 1 mA·cm^(-2).The assembled Li|LiFePO_(4) cell presents outstanding cycling stability(capacity retention of 90%after 400 cycles at 1 C)and good rate performance.The associated pouch cell performs impressive flexibility and safety.This work provides a convenient strategy to achieve stable Li/PVDF interface for high-performance PVDF-based solid state Li metal batteries.

关键词： interfacial modification solid-state batteries composite polymer electrolytes interfacial compatibility lithium dendrite

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A cerium-doped NASICON chemically coupled poly(vinylidene fluoride-hexafluoropropylene)-based polymer electrolyte for high-rate and high-voltage quasi-solid-state lithium metal batteries

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Journal of Energy Chemistry 2022年第10期31卷 311-321,I0007页

作者： Tao Huang Wei Xiong Xue Ye Zhencheng Huang Yuqing Feng Jianneng Liang Shenghua Ye Jishou Piao Xinzhong Wang Yongliang Li Xiangzhong Ren Chao Chen Shaoluan Huang Xiaoping Ouyang Qianling Zhang Jianhong Liu Graphene composite Research Center College of Chemistry and Environmental Engineering.Shenzhen UniversityShenzhen 518060GuangdongChina Institute of information Technology Shenzhen Institute of Information TechnologyShenzhen 518060.GuangdongChina henzhen Eigen-Equation Graphene Technology Co.Ltd Shenzhen 518060Guangdong.China School of Materials Science and Engineering Xiangtan UniversityXiangtan 41105HunanChina

The isolated inorganic particles within composite polymer electrolytes(CPEs) are not correlated to the Li^(+)transfer network,resulting in the polymer dominating the low ionic conductivity of CPEs.Therefore,we developed novel quasi-solid-state CPEs of a Ce-doped Na super ion conductors(NASICON)Na_(1.3+x)Al_(0.3)Ce_(x)Ti_(1.7-x)(PO_(4))_(3)(NCATP) chemically coupled poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP)/Li-bis(trifluoromethanes-ulfonyl)imide(LiTFSI) matrix.A strong interaction between Ce^(3+)from NCATP and TFSI-anion from the polymer matrix contributes to the fast Li+transportation at the interface.The PVDF-HFP/NCATP CPEs exhibit an ionic conductivity of 2.16 × 0^(-3) S cm^(-1) and a Li^(+) transference number of 0.88.A symmetric Li/Li cell with NCATP-integrated CPEs at 0.1 mA cm^(-2) presents outstanding cycling stability over 2000 h at 25℃.The quasi-solid-state Li metal batteries of Li/CPEs/LiFePO_(4) at 2 C after 400 cycles and Li/CPEs/LiCoO_(2) at 0.2 C after 120 cycles deliver capacities of 100 and 152 mAh g^(-1) at 25℃,respectively.

关键词： Quasi-solid-state batteries composite polymer electrolytes High conductivity High-voltage cathode Oxygen vacancies

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Opportunities for ionic liquid-based electrolytes in rechargeable lithium batteries

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Science China Chemistry 2023年第12期66卷 3443-3466页

作者： Xingxing Wang Letao Jin Wenfang Feng Zhibin Zhou Heng Zhang Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Ionic liquids(ILs)have been deemed as promising electrolyte materials for building safer and highly-performing rechargeable lithium batteries,owing to their negligible volatility,low-flammability,and high thermal stability,etc.The profound structural designability of IL cations and anions allows relatively facile regulations of their key physical(e.g.,viscosities,and ionic conductivities)and electrochemical(e.g.,anodic,and cathodic stabilities)properties,and therefore fulfills the critical requirements stipulated by various battery configurations.In this review,a historical overview on the development of ILs for nonaqueous electrolytes is provided,and the correlations between chemical structures and the basic properties of ILs are discussed.Furthermore,the key achievements in the field of IL-based electrolytes are scrutinized,including liquid electrolytes,polymer electrolytes,and composite polymer electrolytes.Based on literature reports and our previous work in this field,possible strategies to improve the performance of IL-based electrolytes and their rechargeable batteries are discussed.The present work not only provides the status quo in the development of IL-based electrolytes but also inspires the structural design of ILs for other kinds of rechargeable batteries(e.g.,sodium,potassium,zinc batteries).

关键词： lithium batteries ionic liquids liquid electrolytes polymer electrolytes composite polymer electrolytes

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A flexible solid polymer electrolyte enabled with lithiated zeolite for high performance lithium battery

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Nano Research 2023年第7期16卷 9443-9452页

作者： Zhiyu Ding Qiming Tang Qi Zhang Penghui Yao Xingjun Liu Junwei Wu Shenzhen Key Laboratory of Advanced Materials Department of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China Maryland Energy Innovation Institute University of MarylandCollege ParkMD 20742USA Department of Chemical and Metallurgical Engineering Aalto UniversityKemistintie 1Aalto FI-00076Finland

Solid-state lithium batteries using composite polymer electrolytes(CPEs)have attracted much attention owing to their higher safety compared to liquid electrolytes and flexibility compared to ceramic electrolytes.However,their unsatisfactory lithium-ion conductivity still limits their development.Herein,a high ion conductive CPE with multiple continuous lithium pathways is designed.This new electrolyte consists of poly(vinylidene fluorideco-hexafluoropropylene)(PVDF-HFP)and lithiated X type zeolite(Li-X),which possesses a high ionic conductivity(1.98×10^(-4)S/cm),high lithium transference number(t_(Li^(+))=0.55),wide electrochemical window(4.7 V),and excellent stability against the lithium anode.Density functional theory(DFT)calculation confirms that the Lewis acid sites in zeolite can graft with N,N-dimethylformamide(DMF)and PVDF-HFP chains,resulting in decreased crystallinity of polymer and providing rapid Li+transmission channels.When used in a full cell,the solid Li|Li-X-3%|LiFePO_(4) cell displays excellent cycling stability and rate performance at room temperature and 60℃.Furthermore,pouch cells with the Li-X-3%electrolyte exhibit brilliant safety under extreme conditions,such as folding and cutting.Thus,this proposed zeolite-PVDF-HFP CPE represents a promising potential in the application of making a safer,higher performing,and flexible solid-state lithium battery.

关键词： solid-state lithium batteries composite polymer electrolytes zeolite poly(vinylidene fluorideco-hexafluoropropylene)(PVDF-HFP) flexible

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Enhanced Electrochemical Performance of Poly(ethylene oxide)composite polymer Electrolyte via Incorporating Lithiated Covalent Organic Framework

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Transactions of Tianjin University 2022年第1期28卷 67-72页

作者： Yuan Yao Yu Cao Gang Li Cheng Liu Zhongyi Jiang Fusheng Pan Jie Sun Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Sinopec Research Institute of Petroleum Processing Beijing 100728China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031China

The lithiated covalent organic framework(named TpPa-SO_(3) Li),which was prepared by a mild chemical lithiation strategy,was introduced in poly(ethylene oxide)(PEO)to produce the composite polymer electrolytes(CPEs).Li-ion can transfer along the PEO chain or across the layer of TpPa-SO_(3) Li within the nanochannels,resulting in a high Li-ion conductivity of3.01×10^(-4)S/cm at 60℃.When the CPE with 0.75 wt.%TpPa-SO_(3) Li was used in the LiFePO_(4)‖Li solid-state battery,the cell delivered a stable capacity of 125 mA·h/g after 250 cycles at 0.5 C,60℃.In comparison,the cell using the CPE without TpPa-SO_(3) Li exhibited a capacity of only 118 mA·h/g.

关键词： Lithiated covalent organic framework composite polymer electrolytes Poly(ethylene oxide) Solid-state lithium-ion batteries

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Synthesis and characterization of mixing soft-segmented waterborne polyurethane polymer electrolyte with room temperature ionic liquid

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Chinese Chemical Letters 2009年第5期20卷 519-522页

作者： Yue Jiao Li Feng Wu Ren Jie Chen School of Chemical Engineering and Environment Beijing Institute of Technology Beijing 100081 China National Development Center for High Technology Green Material Beijing 100081 China

composite polymer electrolytes based on mixing soft-segment waterborne polyurethane （WPU） and 1-butyl-3-methylimidazolium bis[（trifluoromethyl）sulfonyl]imide （BMImTFSI） have been prepared and characterized. The addition of BMImTFSI results in an increase of the ionic conductivity. At high BMImTFSI concentration （BMImTFSI/WPU = 3 in weight ratio）, the ionic conductivity reaches 4.27 × 10^-3 S/cm at 30 ℃. These composite polymer electrolytes exhibit good thermal and electrochemical stability, which are high enough to be applied in lithium batteries.

关键词： composite polymer electrolytes Ionic liquid Waterborne polyurethane Ionic conductivity 1-Butyl-3-methylimidazoliumbis[（trifluoromethyl） sulfonyl]imide

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