Structurally integrated asymmetric polymer electrolyte with stable Janus interface properties for high-voltage lithium metal batteries

Silin Chen; Shunchao Ma; Zhenhua Liu; Yanan Li; Hongxing Yin; Huiyu Song; Min Zhang; Mingyang Xin; Liqun Sun; Yulong Liu; Haiming Xie; Lina Cong

doi:10.1016/j.jcis.2023.01.125

Structurally integrated asymmetric polymer electrolyte with stable Janus interface properties for high-voltage lithium metal batteries

J Colloid Interface Sci. 2023 May 15:638:595-605. doi: 10.1016/j.jcis.2023.01.125. Epub 2023 Jan 27.

Authors

Silin Chen¹, Shunchao Ma², Zhenhua Liu¹, Yanan Li¹, Hongxing Yin¹, Huiyu Song¹, Min Zhang¹, Mingyang Xin¹, Liqun Sun¹, Yulong Liu¹, Haiming Xie³, Lina Cong⁴

Affiliations

¹ National & Local United Engineering Laboratory for Power Battery, Department of Chemistry, Northeast Normal University Changchun, 130024, China.
² State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry Chinese Academy of Sciences, Changchun, 130022, China.
³ National & Local United Engineering Laboratory for Power Battery, Department of Chemistry, Northeast Normal University Changchun, 130024, China. Electronic address: xiehm136@nenu.edu.cn.
⁴ National & Local United Engineering Laboratory for Power Battery, Department of Chemistry, Northeast Normal University Changchun, 130024, China. Electronic address: congln816@nenu.edu.cn.

PMID: 36774873
DOI: 10.1016/j.jcis.2023.01.125

Abstract

Solid-state polymer electrolytes are outstanding candidates for next-generation lithium metal batteries in the realm of high specific energy densities, high safeties and tight contact with electrodes. However, their applications are still hindered by the limitations that no single polymer is electrochemically stable with the oxidizing high-voltage cathode and the highly reductive Li anode, simultaneously. Herein, a bilayer asymmetric polymer electrolyte (SL-SPE) without accessional interface resistance that using poly (ethylene glycol) diacrylate (PEGDA) as a "bridge" to connect the sulfonyl (OS = O)-contained oxidation-tolerated layer and polyether-derived reduction-tolerated layer (SPE), is proposed and synthesized by sequential two-step UV polymerizations. SL-SPE can provide widened electrochemical stability window up to 5 V, while simultaneously deploying a stable Janus interface property. Eventually, the superior high-voltage (4.4 V) cycling durability can be displayed in LiNi_0.6Co_0.2Mn_0.2O₂|SL-SPE|Li batteries. This finding provides a bran-new idea for designing multifunctional polymer electrolytes in the application of solid-state batteries.

Keywords: High-voltage; Interfaces; Lithium metal batteries; Polymer electrolytes; SEI/CEI layers.