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Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-solid-state lithium metal batteries:A Review

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Nano-Micro Letters 2023年第3期15卷 266-297页

作者： Hongmei Liang Li Wang Aiping Wang Youzhi Song Yanzhou Wu Yang Yang Xiangming He Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084People’s Republic of China

solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.

关键词： Polymer Inorganic composite electrolytes All-solid-state lithium metal batteries Fillers Ionic conductivity High voltage

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Highly Efficient Aligned Ion‑Conducting Network and Interface Chemistries for Depolarized all‑solid‑state lithium metal batteries

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Nano-Micro Letters 2024年第5期16卷 102-119页

作者： Yongbiao Mu Shixiang Yu Yuzhu Chen Youqi Chu Buke Wu Qing Zhang Binbin Guo Lingfeng Zou Ruijie Zhang Fenghua Yu Meisheng Han Meng Lin Jinglei Yang Jiaming Bai Lin Zeng Shenzhen Key Laboratory of Advanced Energy Storage Southern University of Science and TechnologyShenzhen 518055People’s Republic of China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055People’s Republic of China SUSTech Energy Institute for Carbon Neutrality Southern University of Science and TechnologyShenzhen 518055People’s Republic of China Department of Mechanical and Aerospace Engineering Hong Kong University of Science and TechnologyKowloon 997077Hong Kong Special Administrative Region of ChinaPeople’s Republic of China HKUST Shenzhen-Hong Kong Collaborative Innovation Research Institute FutianShenzhenPeople’s Republic of China

Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport.solid electrolytes are generally studied as two-dimensional(2D)structures with planar interfaces,showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces.Herein,three-dimensional(3D)architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment.Multiple-type electrolyte films with vertical-aligned micro-pillar(p-3DSE)and spiral(s-3DSE)structures are rationally designed and developed,which can be employed for both Li metal anode and cathode in terms of accelerating the Li+transport within electrodes and reinforcing the interfacial adhesion.The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm^(−2).The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm^(−2)(LFP)and 3.92 mAh cm^(−2)(NCM811).This unique design provides enhancements for both anode and cathode electrodes,thereby alleviating interfacial degradation induced by dendrite growth and contact loss.The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.

关键词： All-solid-state lithium metal batteries Composite solid electrolyte 3D printing Areal capacity Interfacial degradation

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A robust solid electrolyte interphase enabled by solvate ionic liquid for high-performance sulfide-based All-solid-state lithium metal batteries

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Nano Research 2023年第6期16卷 8411-8416页

作者： Jingguang Yi Chong Yan Dan Zhou Li-Zhen Fan Beijing Advanced Innovation Center for Materials Genome Engineering University of Science and Technology BeijingBeijing 100083China School of electrical engineering and automation Luoyang Institute of Science and TechnologyLuoyang 471023China Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuan 030032China

All-solid-state lithium metal batteries(ASSLMBs)that incorporate solid electrolyte(SE)and lithium metal anode suggest considerable potential in addressing the security concerns and energy density limitation of conventional lithium-ion batteries(LIBs).However,the practical application of ASSLMBs is always restricted by the interfacial instability of lithium metal anode/electrolyte and inevitable lithium dendrites propagation in SE.Herein,a solvate ionic liquid is adopted to modify the interface stability of lithium metal anode/electrolyte and inhibit the growth of lithium dendrites via an in-situ formation of a robust solid electrolyte interphase(SEI)on the surface of lithium metal anode.Consequently,the ASSLMBs assembled with Li_(6)PS_(5)Cl(LPSCl)electrolyte,lithium metal anode that protected by robust SEI layer,and LiNbO_(3)@NCM622 cathode exhibit high initial capacity of 126.5 mAh·g^(−1)and improved cycling stability with a capacity retention of 80.3%over 60 cycles at 0.1 C.This work helps to provide a facile route for the design of robust SEI in the application of ASSLMBs.

关键词： All-solid-state lithium metal batteries solvate ionic liquid robust solid electrolyte interphase Li_(6)PS_(5)Cl(LPSCl)electrolyte

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Enhanced ionic conductivity in a novel composite electrolyte based on Gd-doped SnO_(2) nanotubes for ultra-long-life All-solid-state lithium metal batteries

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Journal of Energy Chemistry 2023年第2期77卷 326-337,I0009页

作者： Lugang Zhang Nanping Deng Junbao Kang Xiaoxiao Wang Hongjing Gao Yarong Liu Hao Wang Gang Wang Bowen Cheng Weimin Kang state Key Laboratory of Separation Membranes and Membrane Processes/National Center for International Joint Research on Separation Membranes School of Textile Science and EngineeringTiangong UniversityTianjin 300387China School of Material Science and Engineering Tiangong UniversityTianjin 300387China

all-solid-state electrolytes are exceedingly attractive because of the outstanding inherent safety and energy density compared to liquid electrolytes.Whereas,it is still formidable to simultaneously design solid electrolytes with favorable electrode/electrolyte interface compatibility and high ionic conductivity in a simple and scalable manner.Hence,the oxygen-vacancy-rich Gd-doped SnO_(2) nanotubes(GDS NTs)are innovatively prepared and applied to the electrolyte of All-solid-state lithium metal batteries for the first time.The addition of GDS NTs can validly construct long-range co ntinuous ion transport networks in the poly(ethylene oxide)(PEO)-based system and greatly improve the mechanical properties of the electrolyte.Compared to the PEO-based electrolyte,the composite electrolyte displays a higher lithium ion conductivity of 2.41×10^(-4) S cm^(-1) at 30℃,a higher lithium ion transference number up to 0.62 and a wider electrochemical window of 5 V at 50℃.In addition,the composite electrolyte manifests outstanding compatibility with high-voltage LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)cathode,LiFePO4 cathode and lithium metal anode.The assembled Li/Li symmetric battery exhibits stable Li plating/stripping cycling performance,which can cycle steadily for 1500 h at a capacity of 0.3 mA h cm^(-2).And Li/LiFePO4 battery still maintains a high capacity of 131.54 mA h g^(-1) at 0.5C after 800 cycles,which has a superior capacity retention rate of 93.2%.The obtained novel composite electrolyte has promising application prospects in the field of all-solid-state lithium metal cells.

关键词： All-solid-state lithium metal batteries Gd-doped SnO2 nanotubes Interfacial stability Oxygen vacancies solid-state composite electrolytes

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