Revisiting the Impact of Anion Selection on Sulfur Redox Reaction Kinetics for High Sulfur Loading Lithium–Sulfur Batteries

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-07-10 DOI:10.1002/adma.202507459

Yue Fei, Matthew Li, Zhenfeng Li, Dichang Guan, Wenting Jia, Hao Zhang, Khalil Amine, Ge Li

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引用次数: 0

Abstract

Lithium bis(trifluoromethane)sulfonimide (LiTFSI) is widely used in lithium–sulfur (Li–S) battery electrolytes due to its stability with lithium polysulfides (LiPSs) and moderate compatibility with lithium metal anodes. However, LiTFSI presents environmental concerns due to its association with per‐ and polyfluoroalkyl substances (PFAS), which are environmentally persistent and potentially toxic, raises sustainability concerns. This research also reveals that LiTFSI limits sulfur redox reactions (SRRs), making it less effective than other lithium salts. Additionally, some salts previously considered incompatible with Li‐S systems due to their reactivity with LiPSs are demonstrated to perform effectively. For the first time, a protective, porous cathode electrolyte interphase (CEI) formed in situ through reactions between salt anions and LiPS is reported. The cells delivered a high specific capacity of 1230.8 mAh g−1 at 0.05 C with a sulfur loading of ≈6 mg cm−2, limited lithium anode, maintaining a capacity retention of 76.2% after 100 cycles at 0.1 C. Under harsh conditions, such as high sulfur loading, lean electrolyte conditions (3 µL mg−1), and in anode‐free cells, the cells continued to deliver outstanding capacity. This work provides valuable guidelines for understanding and selecting lithium salts to advance electrolyte design for Li–S batteries.

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阴离子选择对高硫锂硫电池硫氧化还原反应动力学的影响

双（三氟甲烷）磺酰亚胺锂（LiTFSI）由于其与锂多硫化物（LiPSs）的稳定性和与锂金属阳极的适度相容性而被广泛应用于锂硫（li -硫）电池电解质中。然而，LiTFSI由于与全氟烷基和多氟烷基物质（PFAS）相关而引起了环境问题，这些物质具有环境持久性和潜在毒性，引起了可持续性问题。这项研究还表明，LiTFSI限制了硫氧化还原反应（SRRs），使其不如其他锂盐有效。此外，一些以前被认为与Li - S系统不相容的盐，由于它们与LiPSs的反应性，被证明是有效的。首次报道了通过盐阴离子与LiPS的原位反应形成的保护性多孔阴极电解质界面（CEI）。该电池在0.05℃、硫负载≈6 mg cm - 2、有限锂阳极条件下提供了1230.8 mAh g - 1的高比容量，在0.1℃下循环100次后保持了76.2%的容量保留率。在高硫负载、贫电解质条件（3 μ L mg - 1）和无阳极电池等恶劣条件下，电池继续提供出色的容量。这项工作为理解和选择锂盐提供了有价值的指导，以推进锂硫电池的电解质设计。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.