Ca-substituted Na3SbS4 glass–ceramic electrolytes: Achieving high conductivity and excellent interfacial stability

IF 3.8 3区材料科学 Q1 MATERIALS SCIENCE, CERAMICS Journal of the American Ceramic Society Pub Date : 2025-01-15 DOI:10.1111/jace.20379

Yu Shen, Tao Huan, Jingxin Lu, Chengwei Gao, Yongxing Liu, Shixun Dai, Changgui Lin, Xianghua Zhang, Hongli Ma, Xiang Shen, Qing Jiao

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Abstract

Super conductor Na₃SbS₄ has received substantial attention in electrolyte research because of its high ionic conductivity and low grain boundary resistance. A breakthrough in electrochemical stability with good ionic conductivity has yet to be captured. Calcium (Ca) appears as an ideal substitute for sodium (Na) due to its abundance in geological resources, nontoxic properties, and equivalent ionic radius. The proposed Na_3-2_xCa_xSbS₄ glass–ceramic electrolytes were subsequently manufactured using ball milling and heat treatment. The results acquired the maximum ionic conductivity of 1.59 mS cm⁻¹ at room temperature, which reached the commercial use level when compared with the current popular lithium-ion battery. Moreover, calcium ions partially replaced sodium sites while creating massive Na vacancies to maintain charge neutrality, resulting in fast ion transport. Furthermore, a more stable ionic bond Ca–S was formed at the interface, which inhibited additional reactions at the electrolyte–metal interface and demonstrated exceptional cyclic stability, making it a viable electrolyte for solid-state sodium-ion batteries.

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ca取代的Na3SbS4玻璃陶瓷电解质：实现高导电性和优异的界面稳定性

超导体Na3SbS4具有高离子电导率和低晶界电阻等优点，在电解质研究中受到广泛关注。在具有良好离子电导率的电化学稳定性方面尚未取得突破。钙（Ca）因其丰富的地质资源、无毒特性和相当的离子半径而成为钠（Na）的理想替代品。采用球磨和热处理法制备了Na3-2xCaxSbS4玻璃陶瓷电解质。结果表明，室温下离子电导率最高可达1.59 mS cm−1，与目前流行的锂离子电池相比，达到了商用水平。此外，钙离子部分取代钠离子位点，同时产生大量的Na空位以保持电荷中性，从而导致快速离子传输。此外，在界面处形成了更稳定的Ca-S离子键，抑制了电解质-金属界面处的额外反应，并表现出优异的循环稳定性，使其成为固态钠离子电池的可行电解质。

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来源期刊

Journal of the American Ceramic Society 工程技术-材料科学：硅酸盐

CiteScore

7.50

自引率

7.70%

发文量

590

审稿时长

2.1 months

期刊介绍： The Journal of the American Ceramic Society contains records of original research that provide insight into or describe the science of ceramic and glass materials and composites based on ceramics and glasses. These papers include reports on discovery, characterization, and analysis of new inorganic, non-metallic materials; synthesis methods; phase relationships; processing approaches; microstructure-property relationships; and functionalities. Of great interest are works that support understanding founded on fundamental principles using experimental, theoretical, or computational methods or combinations of those approaches. All the published papers must be of enduring value and relevant to the science of ceramics and glasses or composites based on those materials. Papers on fundamental ceramic and glass science are welcome including those in the following areas: Enabling materials for grand challenges[...] Materials design, selection, synthesis and processing methods[...] Characterization of compositions, structures, defects, and properties along with new methods [...] Mechanisms, Theory, Modeling, and Simulation[...] JACerS accepts submissions of full-length Articles reporting original research, in-depth Feature Articles, Reviews of the state-of-the-art with compelling analysis, and Rapid Communications which are short papers with sufficient novelty or impact to justify swift publication.