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solid polymer electrolytes in all-solid-state lithium metal batteries:From microstructures to properties

Journal of Energy Chemistry 2023年第6期81卷 358-378,I0009页

作者： Zongxi Lin Ouwei Sheng Xiaohan Cai Dan Duan Ke Yue Jianwei Nai Yao Wang Tiefeng Liu Xinyong Tao Yujing Liu College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014ZhejiangChina

All-solid-state lithium(Li)metal batteries(ASSLMBs)are considered one of the most promising secondary batteries due to their high theoretical capacity and high safety ***,low room-temperature ionic conductivity and poor interfacial stability are two key factors affecting the practical application of ASSLMBs,and our understanding of the mechanisms behind these key problems from microscopic perspective is still *** this review,the mechanisms and advanced characterization techniques of ASSLMBs are summarized to correlate the microstructures and ***,we summarize the challenges faced by solid polymer electrolytes(SPEs)in ASSLMBs,such as the low roomtemperature ionic conductivity and the poor interfacial ***,several typical improvement methods of polymer ASSLMBs are discussed,including composite SPEs,ultra-thin SPEs,SPEs surface modification and Li anode surface ***,we conclude the characterizations for correlating the microstructures and the properties of SPEs,with emphasis on the use of emerging advanced techniques(e.g.,cryo-transmission electron microscopy)for in-depth analyzing *** influence of the microstructures on the properties is very *** now,it has been difficult for us to understand the microstructures of ***,some recent studies have demonstrated that we have a better understanding of the microstructures of *** we suggest that in situ characterization,nondestructive characterization and sub-angstrom resolution are the key technologies to help us further understand the batteries'microstructures and promote the development of *** potential investigations to understand the microstructures evolution and the batteries behaviors are also prospected to expect further reasonable theoretical guidance for the design of ASSLMBs with ideal performance.

关键词： Lithium metal batteries solid polymer electrolytes Microstructures Properties

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solid polymer electrolytes:Ion conduction mechanisms and enhancement strategies

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Nano Research Energy 2023年第2期2卷 45-88页

作者： Dongmei Zhang Xianglong Meng Wenyan Hou Weihao Hu Jinshan Mo Tianrong Yang Wendi Zhang Qianxiao Fan Lehao Liu Bing Jiang Lihua Chu Meicheng Li State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources School of New EnergyNorth China Electric Power UniversityBeijing 102206China

solid polymer electrolytes(SPEs)possess comprehensive advantages such as high flexibility,low interfacial resistance with the electrodes,excellent film-forming ability,and low price,however,their applications in solid-state batteries are mainly hindered by the insufficient ionic conductivity especially below the melting temperatures,*** improve the ion conduction capability and other properties,a variety of modification strategies have been *** this review article,we scrutinize the structure characteristics and the ion transfer behaviors of the SPEs(and their composites)and then disclose the ion conduction *** ion transport involves the ion hopping and the polymer segmental motion,and the improvement in the ionic conductivity is mainly attributed to the increase of the concentration and mobility of the charge carriers and the construction of fast-ion ***,the recent advances on the modification strategies of the SPEs to enhance the ion conduction from copolymer structure design to lithium salt exploitation,additive engineering,and electrolyte micromorphology adjustion are *** article intends to give a comprehensive,systemic,and profound understanding of the ion conduction and enhancement mechanisms of the SPEs for their viable applications in solid-state batteries with high safety and energy density.

关键词： solid polymer electrolytes ionic conductivity solid-state lithium-ion batteries electrolyte microstructure modification strategies

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Lithium bis(trifluoromethanesulfonyl)imide blended in polyurethane acrylate photocurable solid polymer electrolytes for lithium-ion batteries

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Journal of Energy Chemistry 2021年第11期30卷 485-496,I0011页

作者： Cristian Mendes-Felipe J.C.Barbosa R.Gonsalves D.Miranda C.M.Costa J.L.Vilas-Vilela S.Lanceros-Mendez BCMaterials Basque Center for MaterialsApplications and NanostructuresUPV/EHU Science Park48940 LeioaSpain Macromolecular Chemistry Group(LABQUIMAC) Department of Physical ChemistryFaculty of Science and TechnologyUniversity of the Basque Country(UPV/EHU)Barrio Sarriena s/nE-48940 LeioaSpain Center of Physics University of MinhoCampus of Gualtar4710-057 BragaPortugal Center of Chemistry University of MinhoCampus of Gualtar4710-057 BragaPortugal Ai–School of Technology IPCABarcelosPortugal Ikerbasque Basque Foundation for Science48009 BilbaoSpain

The increased demand of electronic devices promotes the development of advanced and more efficient energy storage devices, such as batteries. Lithium-ion batteries (LIBs) are the most studied battery systems due to their high performance. Among the different battery components, the separator allows the control of lithium ion diffusion between the electrodes. To overcome some drawbacks of liquid electrolytes, including safety and environmental issues, solid polymer electrolytes (SPEs) are being developed. In this work, a UV photocurable polyurethane acrylate (PUA) resin has been blended with lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) up to 30 wt% LiTFSI content to reach a maximum ionic conductivity of 0.0032 mS/cm at room temperature and 0.09 mS/cm at 100 ℃. Those values allowed applying the developed materials as photocurable SPE in Swagelok type Li/C-LiFePO_(4) half-cells, reaching a battery discharge capacity value of 139 mAh.g^(−1) at C/30 rate. Those results, together with the theoretical studies of the discharge capacity at different C-rates and temperatures for batteries with LiTFSI/PUA SPE demonstrate the suitability of the developed photocurable SPE for LIB applications.

关键词： solid polymer electrolytes Photocuring Polyurethane acrylate LiTFSI Li-ion batteries

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Porous garnet as filler of solid polymer electrolytes to enhance the performance of solid-state lithium batteries

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Nano Research 2024年第4期17卷 2663-2670页

作者： Yang Zhang Lei Zhang Peng Guo Chaoyan Zhang Xiaochuan Ren Zhen Jiang Jianjun Song Chuan Shi College of Physics Qingdao UniversityQingdao 266071China Industrial Research Institute of Nonwovens and Technical Textiles College of Textiles and ClothingQingdao UniversityQingdao 266071China Department of Chemistry University of PennsylvaniaPhiladelphiaPA 19104USA

In order to enhance the ionic conductivity of solid polymer electrolytes(SPEs)and their structural rigidity against lithium dendrite during lithium-ion battery(LIB)cycling,we propose porous garnet Li6.4La3Zr2Al0.2O12(LLZO),as the filler to *** porous LLZO with interlinked grains was synthesized via a resol-assisted cationic coordinative co-assembly *** porous structure of LLZO with high specific surface area facilitates the interaction between polymer and filler and provides sufficient entrance for Li^(+)migration into the LLZO ***,the interconnection of LLZO grains forms continuous inorganic pathways for fast Li^(+)migration,which avoid the multiple diffusion for Li^(+)in *** a result,the SPEs with porous LLZO(SPE-PL)show a high ionic conductive of 0.73 mS·cm^(-1) at 30℃ and lithium-ion transference number of *** porous LLZO with uniformly dispersed pores also acts as an ion distributor to regulate ionic *** lithium-symmetrical batteries assembled with SPE-PL show a highly stable Li plating/stripping cycling for nearly 3000 h at 0.1 mA·cm^(-2).The corresponding Li/LiFePO_(4) batteries also exhibit excellent cyclic performance with capacity retention of 75%after nearly 500 *** work brings new insights into the design of conductive fillers and the optimization of SPEs.

关键词： solid polymer electrolytes lithium metal battery porous conductive filler solid state battery

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Exploring porous zeolitic imidazolate frame work-8(ZIF-8)as an efficient filler for high-performance poly(ethyleneoxide)-based solid polymer electrolytes

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Nano Research 2020年第8期13卷 2259-2267页

作者： Zhiwen Lei Jinlai Shen Weide Zhang Qingrong Wang Jun Wang Yonghong Deng Chaoyang Wang Research Institute of Materials Science South China University of TechnologyGuangzhou510640China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou510640China Department of Materials Science and Engineering Academy for Advanced Interdisciplinary StudiesGuangdong Provincial Key Laboratory of Energy Materials for Electric PowerShenzhen518055China

Nano Research volume 13,pages2259–2267(2020)Cite this article 277 Accesses 1 Altmetric Metrics details Abstract The incorporation of inorganic fillers into poly(ethyleneoxide)(PEO)-based solid polymer electrolytes(SPEs)is well known as a low-cost and effective method to improve their mechanical and electrochemical *** zeolitic imidazolate framework-8(ZIF-8)is firstly used as the filler for PEO-based SPEs in this *** to the introduction of ZIF-8,an ionic conductivity of 2.2×10^−5 S/cm(30℃)is achieved for the composite SPE,which is one order of magnitude higher than that of the pure ***-8 also accounts for the broader electrochemical stability window and lithium ion transference number(0.36 at 60℃)of the composite ***,the improved mechanism of ZIF-8 to the composite SPE is investigated by zeta potential and Fourier transform infrared spectrograph *** stability at the composite SPE/lithium interface is greatly *** LiFePO4||Li cells using the composite SPE exhibit high capacity and excellent cycling performance at 60℃,i.e.,85%capacity retention with 111 mA·h/g capacity retained after 350 cycles at 0.5 *** comparison,the cells using the pure PEO show fast capacity decay to 74 mA·h/g maintaining only 68 *** results indicate that the PEO-based SPEs with ZIF-8 are of great promise for the application in solid-state lithium metal batteries.

关键词： zeolitic imidazolate framework inorganic fillers solid polymer electrolytes poly(ethyleneoxide) solid-state lithium metal batteries

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Thermal, Mechanical and Electrical Properties of the PEO-based solid polymer electrolytes Filled by Yttrium Oxide Nanoparticles

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Journal of Wuhan University of Technology(Materials Science) 2012年第3期27卷 495-500页

作者：梁桂杰 Research Center for Materials Science & Engineering Xiangfan University College of Materials Science & Engineering Xi'an Jiaotong University

The novel composite lithium solid polymer electrolytes （SPEs） composed of polyethylene oxide （PEO） matrix and yttrium oxide （Y2O3） nanofillers were prepared by a solution casting method. The crystal morphology of the SPEs was characterized by polarized optical microscope （POM） and wide-angle X-ray diffraction （WAXD）. The induced nucleation and steric hindrance effects of Y2O3 nanofillers result in the increased amount as well as decreased size of PEO spherulites which are closely related to the crystallinity of the SPEs. As the Y2O3 contents increase from 0 wt% to 15 wt%, the crystallinity of the SPEs decreases proportionally. The thermal, mechanical and electrical properties of the SPEs were investigated by thermal gravimetric analysis （TGA）, dynamic mechanical analysis （DMA） and AC impedance method, respectively. The physical properties including thermal, mechanical and electrical performances, depending remarkably on the polymer-filler interactions between PEO and Y2O3 nanoparticles, are improved by different degrees with the increase of Y2O3 contents. The （PEO）21LiI/10 wt%Y2O3 composite SPE exhibits the optimal room-temperature ionic conductivity of 5.95×10-5 Scm-1, which satisfies the requirements of the conventional electrochromic devices.

关键词： solid polymer electrolytes yttrium oxide thermostability mechanical property ionic conductivity

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Ion transport and structural design of lithium-ion conductive solid polymer electrolytes:a perspective

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Materials Futures 2022年第4期1卷 74-92页

作者： Bo Tong Ziyu Song Hao Wu Xingxing Wang Wenfang Feng Zhibin Zhou Heng Zhang Key Laboratory of Material Chemistry for Energy Conversion and Storage Huazhong University of Science and TechnologyWuhan430074 HubeiPeople’s Republic of China

solid polymer electrolytes(SPEs)possess several merits including no leakage,ease in process,and suppressing lithium dendrites *** features are beneficial for improving the cycle life and safety performance of rechargeable lithium metal batteries(LMBs),as compared to conventional non-aqueous liquid ***,the superior elasticity of polymeric material enables the employment of SPEs in building ultra-thin and flexible batteries,which could further expand the application scenarios of high-energy rechargeable *** this perspective,recent progresses on ion transport mechanism of SPEs and structural designs of electrolyte components(*** lithium salts,polymer matrices)are *** addition,key achievements in the field of single lithium-ion conductive SPEs are also outlined,aiming to provide the status quo in those SPEs with high selectivity in cationic ***,possible strategies for improving the performance of SPEs and their rechargeable LMBs are also discussed.

关键词： solid-state lithium metal batteries solid polymer electrolytes single lithium-ion conductor conductive lithium salts polymer matrices

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Quantification and visualization of spatial distribution of dendrites in solid polymer electrolytes

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eScience 2024年第1期4卷 114-122页

作者： Tiancheng Yi Enyue Zhao Yuping He Tianjiao Liang Howard Wang Spallation Neutron Source Science Center Dongguan 523803China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China Neutron Science Platform Songshan Lake Materials LaboratoryDongguan 523808China Institute for Materials Research and Department of Mechanical Engineering Binghamton UniversityBinghamtonNY 13902USA Department of Materials Science and Engineering University of MarylandCollege ParkMD 20742USA

Integrating lithium metal anodes with polymer electrolytes is a promising technology for the next generation high-energy-density rechargeable *** the progress is often hindered by the dendrite growth upon cycling,quantifying three-dimensional(3D)microstructures of dendrites in polymer electrolytes is essential to better understanding of dendrite formation for the development of mitigation *** for 3D quantification and visualization of dendrites,especially those with low Li contents,are rather *** study reports quantitative measurements of the spatial distribution of Li dendrites grown in solid polymer electrolytes using 3D tomographic neutron depth profiling(NDP)with improved spatial resolution,compositional range,and data *** reveal heterogeneous distribution of Li over length scales from tens nanometers to *** most dendrites grow from the plating toward the stripping electrode with dwindling Li quantities,dendrites apparently grown from the Li-stripping electrode are also *** discovery is only possibly due to the unique combination of the high specificity and high sensitivity of the neutron activation analysis of Li isotope.

关键词： Li metal battery solid polymer electrolytes 3D tomographic neutron depth profiling Lithium dendrite

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polymer dispersed ionic liquid electrolytes with high ionic conductivity for ultrastable solid-state lithium batteries

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Carbon Energy 2023年第5期5卷 115-126页

作者： Shengyu Qin Yaping Cao Jianying Zhang Yunxiao Ren Chang Sun Shuoning Zhang Lanying Zhang Wei Hu Meina Yu Huai Yang School of Materials Science and Engineering Beijing Advanced Innovation Center for Materials Genome EngineeringPeking UniversityBeijingPeople's Republic of China Institute for Advanced Materials and Technology University of Science and Technology BeijingBeijingPeople's Republic of China Key Laboratory of polymer Chemistry and Physics of Ministry of Education Peking UniversityBeijingPeople's Republic of China

solid polymer electrolytes(SPEs)have emerged as one of the most promising candidates for building solid-state lithium batteries due to their excellent flexibility,scalability,and interfacial compatibility with ***,the low ionic conductivity and poor cyclic stability of SPEs do not meet the requirements for practical applications of lithium ***,a novel polymer dispersed ionic liquid-based solid polymer electrolyte(PDIL-SPE)is fabricated using the in situ polymerization-induced phase separation(PIPS)*** as-prepared PDIL-SPE possesses both outstanding ionic conductivity(0.74 mS cm^(-1) at 25℃)and a wide electrochemical window(up to 4.86 V),and the formed unique three-dimensional(3D)co-continuous structure of polymer matrix and ionic liquid in PDIL-SPE can promote the transport of lithium ***,the 3D co-continuous structure of PDIL-SPE effectively accommodates the severe volume expansion for prolonged lithium plating and stripping processes over 1000 h at 0.5 mA cm^(-2) under 25℃.Moreover,the LiFePO_(4)//Li coin cell can work stably over 150 cycles at a 1 C rate under room temperature with a capacity retention of 90.6%from 111.1 to 100.7 mAh g^(-1).The PDIL-SPE composite is a promising material system for enabling the ultrastable operation of solid-state lithium-metal batteries.

关键词： high ionic conductivity lithium batteries solid polymer electrolytes solid-state batteries

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A fiber-reinforced solid polymer electrolyte by in situ polymerization for stable lithium metal batteries

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Nano Research 2023年第7期16卷 9259-9266页

作者： Yifan Xu Ruo Zhao Lei Gao Tingsong Gao Wenjuan Wang Juncao Bian Songbai Han Jinlong Zhu Qiang Xu Yusheng Zhao Institute for Advanced Study Shenzhen UniversityShenzhen 518055China Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and DevicesAcademy for Advanced Interdisciplinary StudiesSouthern University of Science and TechnologyShenzhen 518055China Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials Department of Materials Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China School of Materials Science and Engineering Peking UniversityBeijing 100871China

solid polymer electrolytes(SPEs)by in situ polymerization are attractive due to their good interfacial contact with *** reported in situ polymerized SPEs,however,suffer from the low polymerization degree that causes poor mechanical strength,Li dendrite penetration,and performance decay in Li-metal *** highly polymerized SPEs are more stable than lowly polymerized ones,they are restricted by their sluggish long-chain mobility and poor ionic *** this work,a three-dimensional fibrous membrane with ion selectivity was prepared and used as a functional filler for the in situ formed *** obtained SPE has high stability due to its high polymerization degree after the long-term heating *** fibrous membrane plays a vital role in improving the SPE’s *** rich anion-adsorption sites on the fibrous membrane can alleviate the polarization effect and benefit a uniform current distribution at the *** fibrous nanostructure can efficiently interact with the polymeric matrix,providing rich hopping sites for fast Li+***,the obtained SPE enables a uniform Li deposition and long-term cycling performance in Li-metal *** work reported an in situ formed SPE with both high polymerization degree and ionic conductivity,paving the way for designing high-performance SPEs with good comprehensive properties.

关键词： solid polymer electrolytes fibrous solid filler metal-organic frameworks in situ polymerization ion selectivity

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