Enhancing cathode-electrolyte interface stability in high-voltage lithium metal batteries through phase-separated cyano-containing copolymer-based elastomeric electrolytes

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2024-12-21 DOI:10.1016/j.cej.2024.158829
Hyun Soo Kwon, Michael J. Lee, Seung Ho Kwon, Jinseok Park, Hyeonseok Seong, Saehun Kim, Youyoung Byun, Eunji Lee, Nam-Soon Choi, Seung Woo Lee, Bumjoon J. Kim
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Abstract

Solid-state polymer electrolytes (SPEs) are a promising alternative to conventional liquid electrolytes in lithium metal batteries (LMBs). However, their low ionic conductivity and poor oxidation stability hinder the operation of LMBs, particularly when paired with high-voltage, Ni-rich cathodes. To address this challenge, our aim is to integrate the cyano group, known for its ability to enhance oxidation stability through its electron-withdrawing property, into the phase-separated SPEs that exhibit superior ionic conductivity and mechanical properties. Specifically, we synthesize cyano-containing SPEs by incorporating cyanoethyl acrylate (CEA) into an elastomeric electrolyte featuring a bicontinuous structure composed of cyano-containing copolymers and plastic crystals. The phase-separated structure of various SPEs is controlled by adjusting the molar ratio of butyl acrylate (BA) and CEA. At the optimal molar ratio of BA to CEA (specifically, 9:1), this tailored electrolyte shows high ionic conductivity (9.8 × 10−4 S cm−1 at 30 °C) and cycling performance at high cut-off voltage of 4.7 V vs. Li/Li+. The cyano-containing bicontinuous SPEs are expected to play a pivotal role in enhancing oxidation stability and developing robust interfaces consisting of transition metal-anchored framework and inorganic-rich components. These interfaces effectively suppress degradation of cathode structure, thereby achieving high-energy solid-state LMBs.

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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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