Structural engineering and high entropy effect toward improved mechano-electrochemical performance in lithium batteries

IF 11 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Hao-Yu Xu, Rui Wang, Feng-Feng Dong, Zheng Yang, Dong-Yun Li, Yang Xu, Hong-Liang Ge, Ming-Jian Yuan, Qiao-Ling Kang
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Abstract

The inferior structure/electrochemistry stability due to the volume expansion and the less lithium storage active sites of transition metal oxide (TMO) are critical issue hindering their commercialization. The rational design to utilize the combined advantages of both structure and composition is a key strategy to address these challenges. Here, the (FeCoNiMnCrMg)2O3 high entropy oxide (HEO) with different morphologic structures are developed through integrating molecule and microstructure engineering. The morphologic structure of high entropy oxide transforms from solid spheres to multishelled core–shell spheres, and then to hollow spheres, which is governed by a thermally induced non-uniform shrinkage process coupled with Kirkendall effect diffusion due to the different calcination temperature. Even with the incorporation of various metallic ions, the high entropy oxide with a homogeneous single-phase solid solution maintained their shape and uniformity in size due to the ability of metal ions to coexist on the same lattice point. Benefiting from the meticulous control of both compositional and geometric factors, the hollow high entropy oxide exhibited a significantly high specific capacity (1722.1 mAh·g−1 after 200 cycles at 1 A·g−1) and long-life span for lithium storage (2158.7 mAh·g−1 over 900 cycles at 4 A·g−1). The collaborative lattice and consistent volume demonstrated in this study offer significant potential in directing the development of materials for advanced energy storage solutions.

Graphical abstract

结构工程和高熵效应改善锂电池力学电化学性能
过渡金属氧化物(TMO)由于体积膨胀导致的结构/电化学稳定性差和锂存储活性位点少是阻碍其商业化的关键问题。合理的设计利用结构和组合的综合优势是应对这些挑战的关键策略。通过分子工程和微结构工程相结合,制备了具有不同形态结构的(FeCoNiMnCrMg)2O3高熵氧化物(HEO)。高熵氧化物的形态结构由固体球转变为多壳核-壳球,再转变为空心球,这是由不同煅烧温度引起的热诱导非均匀收缩过程和Kirkendall效应扩散所控制的。由于金属离子在同一晶格点上共存的能力,即使加入各种金属离子,具有均匀单相固溶体的高熵氧化物也能保持其形状和尺寸的均匀性。得益于对成分和几何因素的精心控制,空心高熵氧化物在1 a·g−1下循环200次后具有显著的高比容量(1722.1 mAh·g−1)和较长的锂存储寿命(在4 a·g−1下循环900次后具有2158.7 mAh·g−1)。本研究中展示的协同晶格和一致的体积为指导先进储能解决方案材料的开发提供了巨大的潜力。图形抽象
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来源期刊
Rare Metals
Rare Metals 工程技术-材料科学:综合
CiteScore
12.10
自引率
12.50%
发文量
2919
审稿时长
2.7 months
期刊介绍: Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.
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