Sulfhydryl-functionalized COF-based electrolyte  strengthens chemical affinity toward polysulfides in quasi-solid-state Li-S batteries

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Energy Pub Date : 2024-04-17 DOI:10.1002/cey2.544
Linnan Bi, Jie Xiao, Yaochen Song, Tianrui Sun, Mingkai Luo, Yi Wang, Peng Dong, Yingjie Zhang, Yao Yao, Jiaxuan Liao, Sizhe Wang, Shulei Chou
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Abstract

For lithium-sulfur batteries (Li-S batteries), a high-content electrolyte typically can exacerbate the shuttle effect, while a lean electrolyte may lead to decreased Li-ion conductivity and reduced catalytic conversion efficiency, so achieving an appropriate electrolyte-to-sulfur ratio (E/S ratio) is essential for improving the battery cycling efficiency. A quasi-solid electrolyte (COF-SH@PVDF-HFP) with strong adsorption and high catalytic conversion was constructed for in situ covalent organic framework (COF) growth on highly polarized polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) fibers. COF-SH@PVDF-HFP enables efficient Li-ion conductivity with low-content liquid electrolyte and effectively suppresses the shuttle effect. The results based on in situ Fourier-transform infrared, in situ Raman, UV–Vis, X-ray photoelectron, and density functional theory calculations confirmed the high catalytic conversion of COF-SH layer containing sulfhydryl and imine groups for the lithium polysulfides. Lithium plating/stripping tests based on Li/COF-SH@PVDF-HFP/Li show excellent lithium compatibility (5 mAh cm−2 for 1400 h). The assembled Li-S battery exhibits excellent rate (2 C 688.7 mAh g−1) and cycle performance (at 2 C of 568.8 mAh g−1 with a capacity retention of 77.3% after 800 cycles). This is the first report to improve the cycling stability of quasi-solid-state Li-S batteries by reducing both the E/S ratio and the designing strategy of sulfhydryl-functionalized COF for quasi-solid electrolytes. This process opens up the possibility of the high performance of solid-state Li-S batteries.

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巯基官能化 COF 基电解质增强了准固态锂-S 电池对多硫化物的化学亲和力
对于锂硫电池(Li-S 电池)而言,高含量电解质通常会加剧穿梭效应,而贫化电解质则可能导致锂离子电导率下降和催化转化效率降低,因此实现适当的电解质硫比(E/S 比)对于提高电池循环效率至关重要。为了在高极化聚偏氟乙烯-六氟丙烯(PVDF-HFP)纤维上原位生长共价有机框架(COF),我们构建了一种具有强吸附性和高催化转化率的准固体电解质(COF-SH@PVDF-HFP)。COF-SH@PVDF-HFP 可在低含量液态电解质中实现高效锂离子传导,并有效抑制穿梭效应。基于原位傅立叶变换红外光谱、原位拉曼光谱、紫外可见光谱、X 射线光电子学和密度泛函理论计算的结果证实,含有巯基和亚胺基团的 COF-SH 层对多硫化锂具有很高的催化转化率。基于锂/COF-SH@PVDF-HFP/Li 的锂镀层/剥离测试表明锂兼容性极佳(5 mAh cm-2 1400 小时)。组装后的锂-S 电池具有出色的速率(2 C 688.7 mAh g-1)和循环性能(2 C 时为 568.8 mAh g-1,800 次循环后容量保持率为 77.3%)。这是第一份通过降低 E/S 比和准固态电解质巯基官能化 COF 的设计策略来提高准固态锂-S 电池循环稳定性的报告。这一过程为实现固态锂-S 电池的高性能提供了可能。
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来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
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Issue Information Cover Image, Volume 6, Number 10, October 2024 Back Cover Image, Volume 6, Number 10, October 2024 Interface and doping engineering of V2C-MXene-based electrocatalysts for enhanced electrocatalysis of overall water splitting Issue Information
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