Smoothing Li transport via weak Metal-O bonds for improved ionic mobility in lithium lanthanum titanium oxide

IF 10 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Physics Pub Date : 2025-03-17 DOI:10.1016/j.mtphys.2025.101704

Chengran Luo , Yao Shen , Songhe Zhang , Cheng Han , Hongyi Chen

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Abstract

Lithium lanthanum titanate oxide (LLTO) presents significant potential as a solid electrolyte in all-solid-state Li-ion batteries. However, its ionic conductivity requires enhancement for broader applications. In this study, we conducted first-principles calculations to explore the impact of metal doping on LLTO's ionic mobility. LLTO showed uneven ionic diffusion characterized by singular Li-O bonds at certain intermediate states. Ni doping introduced additional electrons into the b₁∗ orbital of the Ti-O anti-bonding, weakening the Ti-O bond and strengthening the Li-O bond. The enhanced Li-O bond facilitated smoother ionic diffusion, reducing the barrier energy to 3.4 × 10⁻⁴ cm²/s for Ni-doped LLTO. Moreover, incorporating various metal dopants in LLTO consistently demonstrated that weaker metal-O bonds contributed to reduced barrier energies. This research underscores the efficacy of diminishing metal-O bonds to significantly boost ionic migration rates in solid-state electrolytes with a perovskite structure.

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通过弱金属- o键平滑Li输运提高镧钛氧化锂离子迁移率

钛酸锂镧氧化物（LLTO）作为全固态锂离子电池的固体电解质具有重要的潜力。然而，为了更广泛的应用，它的离子电导率需要提高。在本研究中，我们通过第一性原理计算来探讨金属掺杂对LLTO离子迁移率的影响。LLTO表现出不均匀的离子扩散，在某些中间态表现为单一的Li-O键。Ni掺杂在Ti-O反键的b1*轨道上引入了额外的电子，削弱了Ti-O键，增强了Li-O键。Li-O键的增强促进了离子扩散，使ni掺杂LLTO的势垒能降低到3.4×10-4 cm2/s。此外，在LLTO中加入各种金属掺杂剂一致表明，较弱的金属- o键有助于降低势垒能。这项研究强调了减少金属- o键在钙钛矿结构的固态电解质中显著提高离子迁移率的功效。

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

Materials Today Physics Materials Science-General Materials Science

CiteScore

14.00

自引率

7.80%

发文量

284

审稿时长

15 days

期刊介绍： Materials Today Physics is a multi-disciplinary journal focused on the physics of materials, encompassing both the physical properties and materials synthesis. Operating at the interface of physics and materials science, this journal covers one of the largest and most dynamic fields within physical science. The forefront research in materials physics is driving advancements in new materials, uncovering new physics, and fostering novel applications at an unprecedented pace.