Coordination Number-Bandgap Relationships at Grain Boundaries in Battery Electrolytes

IF 10.7 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Acta Materialia Pub Date : 2026-10-14 DOI:10.1016/j.actamat.2026.122847

Amith Adoor Cheenady, Krishna Rajan

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引用次数: 0

Abstract

Bandgap alteration at grain boundaries (GBs) in inorganic materials can significantly impact their practical applications. This study probes GBs in four inorganic solid electrolytes (ISEs), γ-Li3PO4, Na3Zr2Si2PO12, Li3YCl6 and Li7La3Zr2O12, and uncovers bandgap-coordination number relationships more complex than those noted in prior investigations. Over-coordination and under-coordination are seen to simultaneously occur in multiple chemical species at GBs, with atoms of the same chemical species exhibiting these modifications to different extents. We find features based on coordination numbers to provide insights into GB bandgap variations in the four ISEs. High-dimensional machine-learned representations of atomistic GB models are used to uncover these GB coordination-bandgap associations, and density functional theory-based density of states evaluations are then used to rationalize the findings.

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电池电解质晶界配位数-带隙关系

无机材料的晶界带隙变化对其实际应用具有重要影响。本研究对γ-Li3PO4、Na3Zr2Si2PO12、Li3YCl6和li7la3zrr2o12这四种无机固体电解质（ISEs）中的GBs进行了研究，发现了比以往研究更复杂的带隙配位数关系。超配位和欠配位同时发生在多种化学物质的GBs中，同一化学物质的原子表现出不同程度的修饰。我们发现了基于协调数的特征，以提供对四个ise中GB带隙变化的见解。使用原子GB模型的高维机器学习表示来揭示这些GB坐标-带隙关联，然后使用基于密度泛函理论的状态密度评估来合理化研究结果。

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

Acta Materialia 工程技术-材料科学：综合

CiteScore

16.10

自引率

8.50%

发文量

801

审稿时长

53 days

期刊介绍： Acta Materialia serves as a platform for publishing full-length, original papers and commissioned overviews that contribute to a profound understanding of the correlation between the processing, structure, and properties of inorganic materials. The journal seeks papers with high impact potential or those that significantly propel the field forward. The scope includes the atomic and molecular arrangements, chemical and electronic structures, and microstructure of materials, focusing on their mechanical or functional behavior across all length scales, including nanostructures.