Deciphering the mechanism of concentrated electrolyte for lithium metal anode via cryogenic electron microscopy
Increasing electrolyte concentration is a typical strategy to boost the stability of lithium (Li) metal anode, yet the fundamental mechanism remains a mystery. By virtue of comprehensive characterization of solid electrolyte interphase (SEI) via cryogenic electron microscopy (Cryo-EM), we revealed the effects of solvation structure in ether-based electrolytes on SEI formation as well as electrochemical performance. The SEI formed in the low-concentration electrolyte (LCE) adopts a Mosaic-type structure with randomly distributed LiCO, which leads to uneven Li deposition and poor cycle stability. The high-concentration electrolyte (HCE) with few free solvent molecules generates an amorphous monolayer SEI, contributing to significantly improved Coulombic efficiency and cycle stability. The addition of non-solvating diluent enables uniform Li deposition on Cu foils in the prepared local high-concentration electrolyte (LHCE), and brings about further enhancement in reversibility and stability. It is correlated with the dual-layer but thinner SEI consisting of an inner amorphous layer and an outer layer made up of mainly crystalline LiSO with high Li conductivity. This work points out the necessity to optimize the SEI structure as well as the solvation structure by altering the salt-to-solvent ratio or adding diluent to modify the viscosity and conductivity of electrolyte system.
National Natural Science Foundation of China ; Shenzhen fundamental research funding["JCYJ20210324115809026","20200925154115001"] ; Shenzhen Science and Technology Program[2019ZT08C044] ; Guangdong Innovative and Entrepreneurial Research Team Program[2022M711467] ; China Postdoctoral Science Foundation[JCYJ20200109141216566] ; null[KQTD20190929173815000]
|WOS Research Area|
Chemistry ; Electrochemistry ; Energy & Fuels ; Materials Science
Chemistry, Physical ; Electrochemistry ; Energy & Fuels ; Materials Science, Multidisciplinary
|WOS Accession No|
|ESI Research Field|
Cited Times [WOS]:0
|Document Type||Journal Article|
|Department||Department of Materials Science and Engineering|
1.School of Materials Science and Engineering,Harbin Institute of Technology,Harbin,150001,China
2.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
3.Graphene Composite Research Center,College of Chemistry and Environmental Engineering,Shenzhen University,Shenzhen,518060,China
4.School of Materials Science and Engineering,Dongguan University of Technology,Dongguan,523808,China
5.Department of Materials Science and Nano Engineering,Rice University,Houston,6100 Main Street,77005,United States
|First Author Affilication||Department of Materials Science and Engineering|
|Corresponding Author Affilication||Department of Materials Science and Engineering|
Li，Menghao,Zhang，Qing,Yang，Xuming,et al. Deciphering the mechanism of concentrated electrolyte for lithium metal anode via cryogenic electron microscopy[J]. JOURNAL OF POWER SOURCES,2023,557.
Li，Menghao.,Zhang，Qing.,Yang，Xuming.,Zhu，Yuanmin.,Cheng，Yifeng.,...&Gu，Meng.(2023).Deciphering the mechanism of concentrated electrolyte for lithium metal anode via cryogenic electron microscopy.JOURNAL OF POWER SOURCES,557.
Li，Menghao,et al."Deciphering the mechanism of concentrated electrolyte for lithium metal anode via cryogenic electron microscopy".JOURNAL OF POWER SOURCES 557(2023).
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