Citation: Wu Chen, Zhou Ying, Zhu Xiaolong, Zhan Minzhi, Yang Hanxi, Qian Jiangfeng. Research Progress on High Concentration Electrolytes for Li Metal Batteries[J]. Acta Physico-Chimica Sinica, ;2021, 37(2): 200804. doi: 10.3866/PKU.WHXB202008044 shu

Research Progress on High Concentration Electrolytes for Li Metal Batteries

Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China

Corresponding author: Qian Jiangfeng, jfqian@whu.edu.cn
Received Date: 16 August 2020
Revised Date: 10 September 2020
Accepted Date: 10 September 2020
Available Online: 16 September 2020
Fund Project: The project was supported by the National Natural Science Foundation of China (21773177) and the Fundamental Research Funds for the Central Universities, China (2042020gf0007)the Fundamental Research Funds for the Central Universities, China 2042020gf0007the National Natural Science Foundation of China 21773177

Improvement in the energy density of conventional lithium-ion batteries (LIBs), based on the intercalation-extraction chemistry of graphite and transition metal layered oxides, has apparently lagged behind the advances in consumer electronics and electric vehicles. Secondary Li-metal batteries (LMBs), utilizing metallic Li as the anode material, have incomparable advantages in terms of energy density due to their high specific capacity (3860 mAh·g^-1) and low redox potential (-3.04 V vs. standard hydrogen electrode) of Li metal. Irrespective of whether Li anodes are coupled with intercalation-type cathodes (e.g. LiFePO₄, LiCoO₂, LiNi_xCo_yMn_zO₂, etc.) or conversion-type cathodes (S, O₂), the energy density of LMBs is much higher than that of traditional LIBs, which should solve the range concern of electric vehicles. However, the intrinsically high reactivity between metallic Li and organic electrolytes could induce the formation of a solid electrolyte interface (SEI). The heterogeneous SEI, consisting of a flexible organic outer layer and a brittle inorganic inner layer, suffers from repeated rupture and regeneration due to infinite volume expansions associated with Li deposition and dissolution reactions. Meanwhile, Li is preferentially deposited on the "hot sites" and is stripped from the root of sediments, resulting in uncontrolled dendrite growth during charging and formation of electrochemically isolated Li ("dead" Li) during discharging. Thus, the Columbic efficiency of Li metal full cells is greatly limited by interfacial side effects and continuous loss of active Li, especially in conventional carbonate-based electrolyte, viz. 1 mol·L^-1 LiPF₆-EC/DEC (ethylene carbonate/diethyl carbonate), which impedes the large-scale employment of Li metal batteries. Recently, novel electrolytes with high or localized-high salt concentrations have attracted considerable attention because of their unique physiochemical properties and excellent electrochemical performance. In high-concentration electrolytes, the reduction in the population of free solvent molecules inhibits irreversible electrolyte decomposition at the electrode-electrolyte interface. In localized-high-concentration electrolytes, the introduction of a dilute reagent retains the desired solvation structure, while improving the physicochemical properties (conductivity and viscosity) of the electrolyte. Herein, we systemically review the latest progress in high-concentration and localized-high-concentration electrolytes for use in Li metal batteries. The solvation chemistry structure, physicochemical properties, and interfacial-stabilizing mechanisms are analyzed in detail, and special attention is devoted to their superior interfacial compatibility with Li metal anodes. Finally, we briefly clarify the current problems associated with the research of high-concentration and localized-high-concentration electrolytes from the viewpoints of basic scientific research and practical applications, and some possible solutions are provided to further pave the way to practical Li metal batteries.
- Li metal battery,
- High concentration electrolyte,
- Localized high concentration electrolyte,
- Electrolyte solvation structure,
- Interfacial property
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沈阳化工大学材料科学与工程学院沈阳 110142