Design Principle of Disordered Rocksalt Type Overlithiated Anode for High Energy Density Batteries

IF 12.2 2区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Materials Horizons Pub Date : 2024-09-13 DOI:10.1039/d4mh00715h

Yufang He, Zhengda He, Bin Ouyang

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Abstract

Rechargeable lithium-ion batteries with high energy density and fast-charging capability are vital for commercial application. Disordered rocksalt (DRX) materials with a cation/anion ratio greater than one, achieved through additional lithium insertion, have emerged as promising high-rate anode candidates. Inspired by the previously reported Li3+xV2O5 (0≤x≤2) anode, a comprehensive search was conducted for all potential redox centers using high-throughput density functional theory (DFT) computations. This study examined 23 redox centers in a prototype formula Li3+xV2O5 (0≤x≤2) with the DRX structure, analyzing aspects such as voltage curve, theoretical capacity, energy density, phase stability, electronic conductivity, and volumetric change during cycling. Promising candidates were identified with redox centers including V, Cr, Nb, Mn, and Fe, marking them as potential anode materials. Additionally, this research revealed the origin of the low voltage in DRX anodes and proposed a method to optimize the average voltage by tuning the relative energies among structures with varying lithium contents. This work provides compositional design principles for new promising DRX anode of LIBs with high energy density, fast-charging capability, and good cycling stability.

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用于高能量密度电池的无序岩盐型过硫化负极的设计原理

具有高能量密度和快速充电能力的可充电锂离子电池对于商业应用至关重要。通过额外的锂插入实现阳离子/阴离子比大于 1 的无序岩盐（DRX）材料已成为有前途的高倍率负极候选材料。受之前报道的 Li3+xV2O5 (0≤x≤2) 负极的启发，我们利用高通量密度泛函理论（DFT）计算对所有潜在的氧化还原中心进行了全面搜索。这项研究考察了具有 DRX 结构的原型式 Li3+xV2O5 (0≤x≤2) 中的 23 个氧化还原中心，分析了电压曲线、理论容量、能量密度、相稳定性、电子电导率和循环过程中的体积变化等方面。研究发现了具有氧化还原中心（包括 V、Cr、Nb、Mn 和 Fe）的有望候选材料，并将其标记为潜在的阳极材料。此外，这项研究还揭示了 DRX 阳极低电压的原因，并提出了一种通过调整不同锂含量结构之间的相对能量来优化平均电压的方法。这项研究为具有高能量密度、快速充电能力和良好循环稳定性的新型 DRX 锂电池负极提供了成分设计原则。

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 Horizons CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

18.90

自引率

2.30%

发文量

306

审稿时长

1.3 months

期刊介绍： Materials Horizons is a leading journal in materials science that focuses on publishing exceptionally high-quality and innovative research. The journal prioritizes original research that introduces new concepts or ways of thinking, rather than solely reporting technological advancements. However, groundbreaking articles featuring record-breaking material performance may also be published. To be considered for publication, the work must be of significant interest to our community-spanning readership. Starting from 2021, all articles published in Materials Horizons will be indexed in MEDLINE©. The journal publishes various types of articles, including Communications, Reviews, Opinion pieces, Focus articles, and Comments. It serves as a core journal for researchers from academia, government, and industry across all areas of materials research. Materials Horizons is a Transformative Journal and compliant with Plan S. It has an impact factor of 13.3 and is indexed in MEDLINE.