Visualization and quantification of Li distribution in garnet solid electrolytes Li6.25La3Zr2Al0.25O12

IF 3.6 2区物理与天体物理 Q2 PHYSICS, APPLIED

Applied Physics Letters Pub Date : 2024-12-09 DOI:10.1063/5.0238020

Zhigang Zhang, Enyue Zhao, Wen Yin, Baotian Wang, Ying Li, Fangwei Wang

引用次数: 0

Abstract

Garnet-type Li7La3Zr2O12 (LLZO) is a promising solid electrolyte for all-solid-state batteries due to its structural stability and high Li+ ionic conductivity, but high-purity LLZO crystallizes in a low-conductivity tetragonal phase at room temperature (RT). Al doping stabilizes the cubic structure, yet its impact on Li+ migration is not fully understood. Using Li6.25La3Zr2Al0.25O12 (LLZAO) as a model, we conducted temperature-dependent neutron powder diffraction (NPD), neutron pair distribution function (nPDF), and density-functional theory (DFT) computations. NPD results, supported by nPDF, show Li+ ions at 24d and 96h sites, excluding 48g. Al at 24d adjusts the distribution of Li, improving ionic conductivity near RT. Maximum Entropy Method analyses indicate a temperature-driven 3D Li diffusion pathway of 24d-96h-96h-24d channels, confirmed by DFT. This work will enhance the understanding of Li diffusion and the optimization of ionic conductivity in garnet-type solid electrolytes.

查看原文本刊更多论文

石榴石固体电解质Li6.25La3Zr2Al0.25O12中Li分布的可视化与定量

石榴石型Li7La3Zr2O12 （LLZO）由于其结构稳定、Li+离子电导率高，是一种很有前途的全固态电池固体电解质，但高纯度LLZO在室温（RT）下以低电导率四方相结晶。Al掺杂稳定了立方结构，但其对Li+迁移的影响尚不完全清楚。以Li6.25La3Zr2Al0.25O12 （LLZAO）为模型，进行了温度相关中子粉末衍射（NPD）、中子对分布函数（nPDF）和密度泛函理论（DFT）计算。NPD结果在nPDF的支持下，显示了24d和96h的Li+离子，不包括48g。Al在24d时调节了Li的分布，提高了rt附近的离子电导率。最大熵法分析表明，24d-96h-96h-24d通道存在温度驱动的3D Li扩散路径，DFT证实了这一点。这项工作将加深对锂在石榴石型固体电解质中的扩散和离子电导率优化的认识。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Applied Physics Letters 物理-物理：应用

CiteScore

6.40

自引率

10.00%

发文量

1821

审稿时长

1.6 months

期刊介绍： Applied Physics Letters (APL) features concise, up-to-date reports on significant new findings in applied physics. Emphasizing rapid dissemination of key data and new physical insights, APL offers prompt publication of new experimental and theoretical papers reporting applications of physics phenomena to all branches of science, engineering, and modern technology. In addition to regular articles, the journal also publishes invited Fast Track, Perspectives, and in-depth Editorials which report on cutting-edge areas in applied physics. APL Perspectives are forward-looking invited letters which highlight recent developments or discoveries. Emphasis is placed on very recent developments, potentially disruptive technologies, open questions and possible solutions. They also include a mini-roadmap detailing where the community should direct efforts in order for the phenomena to be viable for application and the challenges associated with meeting that performance threshold. Perspectives are characterized by personal viewpoints and opinions of recognized experts in the field. Fast Track articles are invited original research articles that report results that are particularly novel and important or provide a significant advancement in an emerging field. Because of the urgency and scientific importance of the work, the peer review process is accelerated. If, during the review process, it becomes apparent that the paper does not meet the Fast Track criterion, it is returned to a normal track.