Cost-Effective and Humid Air-Stable Fluoride Solid Electrolyte with High Ionic Conductivity Induced by Microstructural Modulation

IF 9.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-04-08 DOI:10.1021/acsmaterialslett.5c0002910.1021/acsmaterialslett.5c00029

Xianhui Nie, Meng Lei, Jiulin Hu* and Chilin Li*,

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Abstract

Among halide solid-state electrolytes (SSEs), fluorides show distinct advantages in chemical and electrochemical stability but are plagued by inadequate room-temperature (RT) ionic conductivity. Herein, we propose a cost-effective and humid air-stable fluoride SSE Li₂TiF₆ synthesized by a simple hydrothermal method, exhibiting a high ionic conductivity of 9.69 × 10^–5 S/cm at RT and outstanding humidity tolerance. The enhanced ionic conductivity is demonstrated to originate from microstrain-induced crystal lattice expansion. Furthermore, a stable Li⁺-conductive and intimate interface between halide electrolyte and lithium metal is constructed by introducing a poly(ethylene oxide) protective layer, resulting in the symmetric cell exhibiting a long lifespan with stable cycling over 1000 h at 0.1 mA/cm² as well as the solid-state lithium metal batteries based on the LiFePO₄ cathode reversibly operated for at least 250 cycles at 0.5 C. This work provides fresh perspectives on resolving the cost and various stability issues encountered with halide SSEs.

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微结构调制诱导高离子电导率的低成本湿空气稳定氟化物固体电解质

在卤化物固态电解质（sse）中，氟化物在化学和电化学稳定性方面具有明显的优势，但受到室温（RT）离子电导率不足的困扰。本文采用简单的水热法合成了一种具有成本效益的湿空气稳定氟化物SSE Li2TiF6，在室温下具有9.69 × 10-5 S/cm的高离子电导率和优异的耐湿性。离子电导率的增强源于微应变引起的晶格膨胀。此外，通过引入聚环氧乙烷保护层，在卤化物电解质和锂金属之间构建了一个稳定的Li+导电和亲密的界面。结果表明，对称电池在0.1 mA/cm2下具有超过1000小时的稳定循环寿命，以及基于LiFePO4阴极的固态锂金属电池在0.5 c下可逆运行至少250个循环。这项工作为解决卤化物sse遇到的成本和各种稳定性问题提供了新的视角。

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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.