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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

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Front. Chem. Sci. Eng.    2023, Vol. 17 Issue (10) : 1354-1371    https://doi.org/10.1007/s11705-022-2286-4
REVIEW ARTICLE
Localized high-concentration electrolytes for lithium metal batteries: progress and prospect
Jia-Xin Guo1, Wen-Bo Tang1, Xiaosong Xiong1, He Liu2(), Tao Wang1, Yuping Wu1(), Xin-Bing Cheng1()
1. School of Energy and Environment, Southeast University, Nanjing 211189, China
2. School of Chemistry and Materials Science, Nanjing University of Information Science and Technology, Nanjing 210044, China
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Abstract

With the increasing development of digital devices and electric vehicles, high energy-density rechargeable batteries are strongly required. As one of the most promising anode materials with an ultrahigh specific capacity and extremely low electrode potential, lithium metal is greatly considered an ideal candidate for next-generation battery systems. Nevertheless, limited Coulombic efficiency and potential safety risks severely hinder the practical applications of lithium metal batteries due to the inevitable growth of lithium dendrites and poor interface stability. Tremendous efforts have been explored to address these challenges, mainly focusing on the design of novel electrolytes. Here, we provide an overview of the recent developments of localized high-concentration electrolytes in lithium metal batteries. Firstly, the solvation structures and physicochemical properties of localized high-concentration electrolytes are analyzed. Then, the developments of localized high-concentration electrolytes to suppress the formation of dendritic lithium, broaden the voltage window of electrolytes, enhance safety, and render low-temperature operation for robust lithium metal batteries are discussed. Lastly, the remaining challenges and further possible research directions for localized high-concentration electrolytes are outlined, which can promisingly render the practical applications of lithium metal batteries.
Keywords high-concentration electrolyte      localized high-concentration electrolyte      lithium metal battery      solid electrolyte interphase      dendrite     
Corresponding Author(s): He Liu,Yuping Wu,Xin-Bing Cheng   
Online First Date: 30 March 2023    Issue Date: 07 October 2023
 Cite this article:   
Jia-Xin Guo,Wen-Bo Tang,Xiaosong Xiong, et al. Localized high-concentration electrolytes for lithium metal batteries: progress and prospect[J]. Front. Chem. Sci. Eng., 2023, 17(10): 1354-1371.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2286-4
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I10/1354
Fig.1  Schematic diagrams of the electrolyte structures: (a) high-concentration electrolyte, (b) conventional-concentration electrolyte, and (c) LHCE.
Fig.2  (a) Schematics showing the Li self-corrosion process in 1 mol·L–1 Li bis(trifluoromethanesulfonyl)imide/1,3-dioxolane-1,2-dimethoxyethane electrolyte (left) and 4 mol·L–1 Li bis(trifluoromethanesulfonyl)imide/1,3-dioxolane-1,2-dimethoxyethane electrolyte (right). Reprinted with permission from Ref. [72], copyright 2020, American Chemical Society. (b) Schematics of deposited Li in the baseline carbonate electrolyte and Li bis(trifluoromethanesulfonyl)imide-acetonitrile-vinylene carbonate electrolyte. Reprinted with permission from Ref. [85], copyright 2020, Wiley-VCH Verlag. (c) Schematics of solvation structure and SEI formed in dimethyl carbonate-based LHCE and 1,2-dimethoxyethane-based LHCE. Reprinted with permission from Ref. [87], copyright 2021, American Chemical Society. (d) Scanning electron microscope (SEM) images of pristine cathode and the cycled cathodes using conventional-concentration electrolyte, high-concentration electrolyte, and LHCE-2 electrolytes. Reprinted with permission from Ref. [100], copyright 2022, Royal Society of Chemistry.
Fig.3  (a) Cycling stability and efficiency with 1.2 mol·L–1 LiFSI/dimethyl carbonate-bis(2,2,2-trifluoroethyl) ether at C/2 charge and 2 C discharge rates. Reprinted with permission from Ref. [58], copyright 2018, Wiley-VCH Verlag GmbH. (b) SEM images of aluminum foils after tests in the high-concentration electrolyte and the LHCE. Reprinted with permission from Ref. [110], copyright 2018, Elsevier. (c) Linear sweep voltammetry (LSV) comparison results of four electrolytes on aluminum foil with a scan rate of 1 mV·s–1. Reprinted with permission from Ref. [115], copyright 2020, American Chemical Society. (d) LSV curves in a three-electrode cell at a scanning rate of 0.5 mV·s–1 and atomic force microscope images of the aluminum foil in different electrolytes. Reprinted with permission from Ref. [116], copyright 2020, American Chemical Society. (e) Cost comparison of different fluoride diluents. Reprinted with permission from Ref. [118], copyright 2022, Elsevier. (f) LSV curves of various electrolytes (scan rate: 1 mV·s–1). Reprinted with permission from Ref. [118], copyright 2022, Elsevier. (g) Schematic illustration of the interphases formed between Li metal anodes and CNE-NI electrolytes. Reprinted with permission from Ref. [119], copyright 2022, Wiley.
Fig.4  (a) Flammability tests of the control electrolyte of 1 mol·L–1 Li hexafluorophosphate/ethylenecarbonate + diethyl carbonate, and the highly concentrated 5 mol·L–1 LiFSI/triethyl phosphate electrolyte. Reprinted with permission from Ref. [131], copyright 2018, Royal Society of Chemistry. (b) Function mechanism of functional LHCEs. Reprinted with permission from Ref. [134], copyright 2022, Wiley. (c) Flammability test of carbonate electrolyte and LiFSI/triethyl phosphate-1,1,2,2-tetrafuoroethyl-2’,2’,2’-trifuoroethyl + 2-fluoropyridine. Reprinted with permission from Ref. [137], copyright 2022, American Chemical Society. (d) Conceptual illustrations of full cell structures and the material design of Li ion batteries and LMBs. Reprinted with permission from Ref. [138], copyright 2020, Elsevier.
Fig.5  (a) Flammability tests of the ionic-liquid electrolyte and a conventional organic electrolyte consisting of 1 mol·L–1 Li hexafluorophosphate in ethylene carbonate/dimethyl carbonate (1:1 by vol). Reprinted with permission from Ref. [140], copyright 2020, Wiley-VCH Verlag GmbH. (b) Photographs of ignition tests of glass fibers saturated with different electrolytes. Reprinted with permission from Ref. [142], copyright 2022, Elsevier.
Fig.6  (a) Rate performance at the ultra-low temperature of –70 °C. Reprinted with permission from Ref. [146], copyright 2019, Wiley-VCH GmbH. (b) Ionic conductivity of two electrolytes at different temperatures. Reprinted with permission from Ref. [147], copyright 2021, Wiley-VCH Verlag. (c) The key factors determining the Li cycling performance of LHCE versus high-concentration electrolyte at 5–60 °C. Reprinted with permission from Ref. [148], copyright 2022, Elsevier. (d) Li||LiNi0.5Mn0.3Co0.2O2 cell powers LED bulbs at –40 °C. Reprinted with permission from Ref. [149], copyright 2022, American Chemical Society.
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