Sulfone electrolyte based quasi-solid-state high-voltage lithium metal batteries enabled by component design and interfacial engineering

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Qingru Zhou , Zhouyu Huang , Tianqi Yang , Haiyuan Zhang , Xiayin Yao , Wenkui Zhang , Hui Huang , Yang Xia , Xinyong Tao , Jun Zhang
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Abstract

Sulfone-based electrolyte (SL) as a novel type electrolyte for lithium-ion batteries (LIBs) has attracted increasing attention due to its exceptional high-voltage stability and flame retardancy. However, the polar thionyl groups in sulfone lead to continuous reaction with lithium (Li) metal, and high viscosity of sulfone could decrease its Li+ ionic conductivity, which obstructs further application of SL in Li metal batteries (LMBs). Herein, the methylenebisacrylamide (MBA) crosslinked SL, fluorinated ethylene carbonate (FEC) based quasi-solid-state electrolyte (MSFE) was designed to address above problems. By introducing FEC to passivate metallic Li and 1H,1H,5H-octafluoropentyl-1,1,2,2-tetrafluoroethyl ether (OTE) as diluent to decrease viscosity of electrolyte, MSFE exhibits a high ionic conductivity of 1.77 × 10−3 S cm−1 and wide electrochemical stability window up to 5.6 V. Therefore, LiCoO2/MSFE/Li (LCO/MSFE/Li) batteries show a high capacity retention of 95.7 % after 100 cycles under 0.2C. Moreover, formation mechanism and kinetic evolution of the hybrid EEI is revealed via density functional theory (DFT) calculations and in-situ galvanostatic electrochemical impendence spectra (IS-GEIS) coupled with distribution relax time (DRT) technology. Well-formed hybrid EEI prevents the structural degradation of LCO materials and induces uniform deposition of Li-ion to inhibit formation of Li dendrites. This work provides a new insight towards high energy density in-situ polymerized solid LMBs.

Abstract Image

Abstract Image

基于砜电解质的准固态高压锂金属电池的组件设计和界面工程实现
砜基电解质(SL)作为一种新型的锂离子电池电解质,因其优异的高压稳定性和阻燃性而受到越来越多的关注。然而,砜中极性亚硫基导致其与锂金属的连续反应,且砜的高粘度会降低其Li+离子电导率,阻碍了SL在锂金属电池(lbs)中的进一步应用。针对上述问题,设计了基于亚甲基双丙烯酰胺(MBA)交联SL、氟化碳酸乙烯(FEC)的准固态电解质(MSFE)。通过引入FEC钝化金属Li和1H,1H, 5h -辛氟戊基-1,1,2,2-四氟乙醚(OTE)作为稀释剂来降低电解质粘度,MSFE具有1.77 × 10−3 S cm−1的高离子电导率和高达5.6 V的宽电化学稳定窗口。因此,在0.2C下循环100次后,LiCoO2/MSFE/Li (LCO/MSFE/Li)电池的容量保持率高达95.7% %。此外,通过密度泛函理论(DFT)计算和原位恒流电化学阻抗谱(is - geis)结合分布松弛时间(DRT)技术揭示了混合EEI的形成机理和动力学演化。结构良好的杂化EEI阻止了LCO材料的结构降解,诱导Li离子均匀沉积,抑制了Li枝晶的形成。这项工作为高能密度原位聚合固体lmb提供了新的思路。
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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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