A 'Seat-Squatting' Strategy via Lithium Substitution to Suppress Fe-Migration in Na layered Oxide Cathodes

IF 32.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yaoshen Niu, Zilin Hu, Huican Mao, Lin Zhou, Liguang Wang, Xiaobing Lou, Bo Zhang, Dongdong Xiao, Yang Yang, Feixiang Ding, Xiaohui Rong, Ju-Ping Xu, Wen Yin, Nian Zhang, Zhiwei Li, Yaxiang Lu, Bingwen Hu, Jun Lu, Ju Li, Yong-Sheng Hu
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引用次数: 0

Abstract

Na-ion batteries (NIBs) are emerging as a promising alternative to Li-ion batteries (LIBs). To align with sustainability principles, the design of electrode materials must incorporate considerations for abundant and environmentally friendly elements, such as redox-active Fe. Despite its appeal, the enduring challenge of Fe migration in layered cathodes remains inadequately addressed over decades. Here, we propose a "seat-squatting" strategy via Li-substitution to fundamentally suppress Fe migration. Li is strategically introduced to migrate first, occupying available migration sites without inducing structural damage and effectively raising the activation energy for Fe migration. Experimental and theoretical validation using O3-Na0.83Li0.17Fe0.33Mn0.5O2 (NaLFM) demonstrates a robust suppression of irreversible Fe migration. As a result, the NaLFM cathode delivers enhanced structural and electrochemical cycling stability. This work illustrates a compelling strategy to curb irreversible Fe migration in NIBs, offering a pathway for the development of stable and cost-effective layered oxides based on Fe redox centers.
通过锂置换抑制 Na 层氧化物阴极中的铁迁移的 "座次 "策略
作为锂离子电池(LIB)的替代品,纳离子电池(NIB)正在崭露头角。为了符合可持续发展原则,电极材料的设计必须考虑到丰富的环保元素,如具有氧化还原作用的铁。尽管层状阴极具有吸引力,但几十年来,层状阴极中铁迁移这一持久挑战仍未得到充分解决。在这里,我们提出了一种通过锂置换来从根本上抑制铁迁移的 "坐席 "策略。锂被策略性地引入并首先迁移,在不引起结构破坏的情况下占据可用的迁移位点,并有效提高铁迁移的活化能。使用 O3-Na0.83Li0.17Fe0.33Mn0.5O2 (NaLFM) 进行的实验和理论验证表明,这种方法能有效抑制铁的不可逆迁移。因此,NaLFM 阴极具有更高的结构和电化学循环稳定性。这项工作展示了一种抑制非氧化物负极中铁不可逆迁移的有力策略,为开发基于铁氧化还原中心的稳定且经济高效的层状氧化物提供了一条途径。
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来源期刊
Energy & Environmental Science
Energy & Environmental Science 化学-工程:化工
CiteScore
50.50
自引率
2.20%
发文量
349
审稿时长
2.2 months
期刊介绍: Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).
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