Vertically Heterostructured Solid Electrolytes for Lithium Metal Batteries

He, Fei; Hu, Zhenglin; Tang, Wenjing; Wang, Aoxuan; Wen, Bohua; Zhang, Lan; Luo, Jiayan

doi:10.1002/adfm.202201465

Cited by 27 publications

(16 citation statements)

References 184 publications

(172 reference statements)

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“…Meanwhile, combining anions with the fillers can diminish the shielding effect of anions on the positive charges of polymers and effectively stabilize the polymers at high voltage. Furthermore, rational design of polymer and inorganic Li + conductors can inhibit the direct contact of unstable interface and improve the compatibility with Li and high-voltage cathode [ 48 ]. Specifically, most polymers are stable at the Li anode but poor at the high-voltage cathode, whereas certain inorganic oxides and sulfides are the exact reverse.…”

Section: Key Issues In the Development Of Piesmentioning

confidence: 99%

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries: A Review

Liang

Wang

et al. 2023

Nano-Micro Lett.

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Highlights The current issues and recent advances in polymer/inorganic composite electrolytes are reviewed. The molecular interaction between different components in the composite environment is highlighted for designing high-performance polymer/inorganic composite electrolytes. Inorganic filler properties that affect polymer/inorganic composite electrolyte performance are pointed out. Future research directions for polymer/inorganic composite electrolytes compatible with high-voltage lithium metal batteries are outlined. Abstract 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.

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Section: Key Issues In the Development Of Piesmentioning

confidence: 99%

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries: A Review

Liang

Wang

et al. 2023

Nano-Micro Lett.

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“…[99] In addition to the single-layered designs, combining different electrolytes to assemble layered structures is another practical method to improve the ion-conduction behavior. [16,100,101] More details for recent advanced composite polymer solid electrolytes with good ionic conductivity in different structural designs are discussed below.…”

Section: Composite Solid Electrolytesmentioning

confidence: 99%

Advanced Composite Solid Electrolytes for Lithium Batteries: Filler Dimensional Design and Ion Path Optimization

Zheng

et al. 2023

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organic liquid electrolytes hinder lithium batteries in achieving higher energy density, longer working life, and safer performance. [12,13] Solid electrolytes not only improve the long-term thermal and electrochemical stabilities but also obviate the need for separators and increase the energy density. [14][15][16][17] From these concerns, solid electrolytes are regarded as a potential substituent to improve the cycle performance of lithium batteries.Solid electrolytes are generally categorized as solid polymer electrolytes, inorganic solid electrolytes, and composite solid electrolytes. [16,18,19] Solid polymer electrolytes, such as poly(ethylene oxide) (PEO) and poly(vinylidene fluoride) (PVDF), are favored for their chemical stability, low density, low cost, processability, and wettability. [20][21][22][23] However, the applications are restricted by their low ionic conductivity at room temperature (typically from 10 −6 to 10 −5 S cm −1 ). Therefore, much research has been devoted to synthesizing solid polymer electrolytes with high ionic conductivity via increasing free volume and constructing fast transport paths, such as applying covalent organic framework-based polymer, [24,25] single lithium-ion-conducting polymer, [26,27] crosslinked polymer network, [28,29] and adding plasticizers. [30,31] Inorganic solid electrolytes, such as Li 7 La 3 Zr 2 O 12 (LLZO, garnet-type) and Li 0.33 La 0.56 TiO 3 (LLTO, perovskite-type), are single-ion conductors with superior lithium-ion conductivity (typically from 10 −4 to 10 −2 S cm −1 ). [32][33][34][35] However, inorganic solid electrolytes usually have a defect of high interfacial contact resistance because of the poor wettability at the electrode and electrolyte interface. [36,37] Moreover, recent studies have proved that the ion transport at the interface and the ionic conductivity of electrolytes are both essential to maintain a stable interface between electrode and electrolyte. [38][39][40] Therefore, constructing composite solid electrolytes by utilizing the advantages of both polymeric and inorganic materials is generally viewed as a practicable solution for nextgeneration lithium batteries. [16,41,42] Many recent studies have shown that the ion-conduction behavior is significantly influenced by the filler structures in a polymer/salt matrix, in which the effect is determined by the natural characteristics of the fillers and the interaction Composite solid electrolytes are considered to be the crucial components of all-solid-state lithium batteries, which are viewed as the next-generation energy storage devices for high energy density and long working life. Numerous studies have shown that fillers in composite solid electrolytes can effectively improve the ion-transport behavior, the essence of which lies in the optimization of the ion-transport path in the electrolyte. The performance is closely related to the structure of the fillers and the interaction between fillers and other electrolyte components including polymer matrices and lithium salts. In this rev...

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“…XPS analysis shows that lithium fluoride and lithium alkoxides species dominate at PEO-lithium bis(trifluoromethanesulfonyl) imide (LiTFSI)/Li metal interface. [136] In contrast, poly(acrylonitrile) (PAN), [137,138] poly(N-methyl-malonic amide) (PMA), [139] polyvinylidene fluoride hexafluoropropylene (PVdF-HFP), [140] etc. form continuously growing and resistive interfacial layers with Li metal.…”

Section: Electrochemical Instability Of Solid Electrolytementioning

confidence: 99%

Anode Interfacial Issues in Solid‐State Li Batteries: Mechanistic Understanding and Mitigating Strategies

Wang

Chen

et al. 2023

Energy & Environ Materials

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All‐solid‐state Li metal batteries (ASSLBs) using inorganic solid electrolyte (SE) are considered promising alternatives to conventional Li‐ion batteries, offering improved safety and boosted energy density. While significant progress has been made on improving the ionic conductivity of SEs, the degradation and instability of Li metal/inorganic SE interfaces have become the critical challenges that limit the coulombic efficiency, power performance, and cycling stability of ASSLBs. Understanding the mechanisms of complex/dynamic interfacial phenomena is of great importance in addressing these issues. Herein, recent studies on identifying, understanding, and solving interfacial issues on anode side in ASSLBs are comprehensively reviewed. Typical issues at Li metal/SE interface include Li dendrite growth/propagation, SE cracking, physical contact loss, and electrochemical reactions, which lead to high interfacial resistance and cell failure. The causes of these issues relating to the chemical, physical, and mechanical properties of Li metal and SEs are systematically discussed. Furthermore, effective mitigating strategies are summarized and their effects on suppressing interfacial reactions, improving interfacial Li‐ion transport, maintaining interfacial contact, and stabilizing Li plating/stripping are highlighted. The in‐depth mechanistic understanding of interfacial issues and complete investigations on current solutions provide foundations and guidance for future research and development to realize practical application of high‐performance ASSLB.

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Vertically Heterostructured Solid Electrolytes for Lithium Metal Batteries

Cited by 27 publications

References 184 publications

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries: A Review

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries: A Review

Advanced Composite Solid Electrolytes for Lithium Batteries: Filler Dimensional Design and Ion Path Optimization

Anode Interfacial Issues in Solid‐State Li Batteries: Mechanistic Understanding and Mitigating Strategies

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