Proton-exchange induced reactivity in layered oxides for lithium-ion batteries

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-11-13 DOI:10.1038/s41467-024-53731-2
Panpan Xu, Xingyu Guo, Binglei Jiao, Jinxing Chen, Minghao Zhang, Haodong Liu, Xiaolu Yu, Maura Appleberry, Zhenzhen Yang, Hongpeng Gao, Fan Yang, Xuefei Weng, Yanbin Shen, Jing Gu, Ying Shirley Meng, Christopher Brooks, Shyue Ping Ong, Zheng Chen
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Abstract

LiNixCoyMn1-x-yO2 (0 < x, y < 1, NCM) is the dominant positive material for the state-of-the-art lithium-ion batteries. However, the sensitivity of NCM materials to moisture makes their manufacturing, storage, transportation, electrode processing and recycling complicated. Although it is recognized that protons play a critical role in their structure stability and performance, proton exchange with Li+ in NCM materials has not been well understood. Here, we employ advanced characterizations and computational studies to elucidate how protons intercalate into the layered structure of NCM, leading to the leaching of Li+ and the formation of protonated NCM. It is found that protonation facilitates cation rearrangement and formation of impurity phases in NCM, significantly deteriorating structural stability. The adverse effects induced by protons become increasingly pronounced with a higher Ni content in NCM. Through a comprehensive investigation into the thermodynamics and kinetics of protonation, we discover that Li deficiencies in NCM materials can be resolved via solution process in the presence of Li+ ions and controlled proton concentration. The underlying mechanism of relithiation is further explored through materials characterizations and kinetics modeling. This work provides crucial insights into controlling structural and compositional defects of Li-ion battery positive material in complicated processing environment.

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用于锂离子电池的层状氧化物中的质子交换诱导反应性
LiNixCoyMn1-x-yO2 (0 < x, y < 1, NCM) 是最先进的锂离子电池的主要正极材料。然而,NCM 材料对水分的敏感性使其制造、储存、运输、电极加工和回收变得复杂。虽然人们认识到质子对其结构稳定性和性能起着至关重要的作用,但对 NCM 材料中质子与 Li+ 的交换还不甚了解。在此,我们采用先进的表征和计算研究来阐明质子如何插层到 NCM 的层状结构中,从而导致 Li+ 的沥滤和质子化 NCM 的形成。研究发现,质子化促进了 NCM 中阳离子的重排和杂质相的形成,从而大大降低了结构的稳定性。NCM 中的镍含量越高,质子诱发的不利影响就越明显。通过对质子化热力学和动力学的全面研究,我们发现 NCM 材料中的锂缺陷可在 Li+ 离子存在和质子浓度受控的情况下通过溶液过程解决。通过材料表征和动力学建模,我们进一步探索了再锂化的基本机制。这项工作为在复杂的加工环境中控制锂离子电池正极材料的结构和组成缺陷提供了重要见解。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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