Hydrogen Bond Reconstruction Maneuver in Eutectic Electrolyte Enables Ultralong-Lifespan Zinc-Ion Batteries.

IF 15.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-10-17 DOI:10.1021/jacs.5c12021

Xuemei Zhang,Qiang Tang,Hang Luo,Yanling Xu,Sicheng Miao,Shuyang Zhou,Changhaoyue Xu,Ye Jia,Qiujie He,Jianan Peng,Liang He,Yingze Song,Yun Zhang,Wenlong Cai

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引用次数: 0

Abstract

Eutectic electrolytes (EEs) serve as a kind of ionic liquid-analogue electrolytes, newly emerging due to their low cost, high stability, biodegradability, nonflammability, and easy preparation properties. The commonly used quaternary ammonium salts play the role of acceptors to form hydrogen bonds (HBs), while the inorganic anions are mostly anchored. Herein, a new type of choline-chloride-based EE was prepared by reshaping the HB donor-acceptor identity to unconstrain chloride anions. Multiple spectral characterizations combined with theoretical analysis confirm the existence of reconstructed HBs and the formation of an anion-dominated solvation structure. Consequently, an organic-inorganic hybrid solid electrolyte interphase film was created on the Zn surface, realizing dendrite-free Zn anodes and achieving an ultralong lifespan of 18175 h (∼2.07 years) of highly reversible Zn plating/stripping performance at a current density of 0.5 mA cm-2, even a super high cumulative capacity of 42 Ah cm-2 at 20 mA cm-2. Furthermore, the assembled Zn || AC@I2 pouch cell shows stable rate and cycling electrochemical properties. This research sheds new light on developing EEs for high-safety and practical zinc-ion batteries.

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共晶电解液中氢键重构机动实现超长寿命锌离子电池。

共晶电解质是一种新型离子液体模拟电解质，具有成本低、稳定性高、可生物降解、不易燃、制备方便等特点。常用的季铵盐作为受体形成氢键（HBs），而无机阴离子大多是锚定的。本文通过重塑HB的供体-受体身份以解除氯离子的约束，制备了一种新型的氯化胆碱基EE。多重光谱表征结合理论分析证实了重构HBs的存在和阴离子为主的溶剂化结构的形成。因此，在Zn表面形成了有机-无机杂化固体电解质界面膜，实现了无枝晶Zn阳极，并在0.5 mA cm-2电流密度下实现了18175 h（~ 2.07年）的高可逆Zn电镀/剥离性能，甚至在20 mA cm-2电流密度下实现了42 Ah cm-2的超高累积容量。此外，组装的锌|| AC@I2袋状电池具有稳定的速率和循环电化学性能。本研究为开发高安全性、实用型锌离子电池的EEs提供了新的思路。

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

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.