Non-fluorinated electrolytes with micelle-like solvation for ultra-high energy density lithium metal batteries

IF 9.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2024-10-03 DOI:10.1016/j.chempr.2024.09.005

Rui Qiao, Yan Zhao, Shijie Zhou, Huijun Zhang, Fuzhu Liu, Tianhong Zhou, Baoyu Sun, Hao Fan, Chao Li, Yanhua Zhang, Feng Liu, Xiangdong Ding, Jang Wook Choi, Ali Coskun, Jiangxuan Song

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引用次数: 0

Abstract

Electrolyte engineering plays a critical role in enabling lithium (Li) metal batteries. However, the simultaneous realization of anion-rich solvation structure and high ionic conductivity of electrolytes via solvation structure design remains challenging. Here, we report a low-cost, non-fluorinated electrolyte with a micelle-like solvation structure by introducing amphiphilic n-butyl methyl ether (MNBE) into Li bis(fluorosulfonyl)imide (LiFSI)/1,2-dimethoxyethane (DME) for stable Li metal batteries (LMBs). MNBE can effectively promote Li⁺-FSI⁻ coordination through steric crowding. Meanwhile, the inert alkyl chains of MNBE can mitigate the reaction between electrolyte and Li metal due to their lithiophobicity. Specifically, the micelle-like, non-fluorinated electrolyte exhibits an ionic conductivity as high as 12.55 mS cm⁻¹, and its anion-rich solvation structure promotes the formation of LiF-rich solid-electrolyte interphase. We constructed a 7.3 Ah Li||NMC811 pouch cell employing this electrolyte under harsh conditions, exhibiting ultra-high specific energy of 503.7 Wh kg⁻¹ with impressive cycling stability of 84.1% capacity retention after 100 cycles.

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用于超高能量密度锂金属电池的胶束状溶解的无氟电解质

电解质工程在实现锂（Li）金属电池方面发挥着至关重要的作用。然而，通过溶解结构设计同时实现电解质的富阴离子溶解结构和高离子电导率仍然具有挑战性。在此，我们通过在双氟磺酰亚胺锂（LiFSI）/1,2-二甲氧基乙烷（DME）中引入两亲性正丁基甲基醚（MNBE），报告了一种具有胶束状溶解结构的低成本无氟电解质，可用于制造稳定的锂金属电池（LMB）。MNBE 可通过立体拥挤有效促进 Li+-FSI- 配位。同时，MNBE 的惰性烷基链具有疏锂性，可减轻电解质与锂金属之间的反应。具体来说，胶束状非氟化电解质的离子电导率高达 12.55 mS cm-1，其富含阴离子的溶解结构促进了富含 LiF 的固体-电解质间相的形成。我们在苛刻的条件下利用这种电解质构建了一个 7.3 Ah 的锂||NMC811 袋式电池，显示出 503.7 Wh kg-1 的超高比能量和令人印象深刻的循环稳定性，100 次循环后容量保持率为 84.1%。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.