Coherent Strain-Inhibiting Phase Construction of Lithium-Rich Manganese-Based Oxide Toward High Mechanochemical Stability

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2025-01-21 DOI:10.1021/jacs.4c11385
Zhou Xu, Xingzhong Guo, Xuemei Zeng, Junxiang Liu, Jingran Yin, Minglu Ren, Junzhang Wang, Tengteng Qin, Zhizhen Zhang, Luxi Li, Khalil Amine, Yifei Yuan, Tongchao Liu
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Abstract

A layered lithium-rich manganese-based oxide cathode, containing Rm (LiTMO2, TM = Mn, Ni, Co) and C2/m (Li2MnO3) nanodomains, utilizes both transition metals and oxygen redox to yield substantial energy density. However, the inherent heterogeneous nature and distinct nanodomain redox chemistries of layered lithium-rich oxides will inevitably cause pernicious lattice strain and structural displacement, which can hardly be eliminated by conventional doping or coating strategies and result in accelerated performance decay. Herein, we incorporate a strain-inhibiting perovskite phase coherently grown within the layered structure to effectively restrain the displacement and lattice strain during uneven Li-ion extraction. The enhanced mechanochemical stability of the designed cathode benefits the persistent structure and reversible oxygen redox, thereby achieving high initial Coulombic efficiency and stable cycling and voltage profiles. Our approach of lattice engineering alleviates the strain and displacement caused by inhomogeneous reactivity between heterogeneous nanodomains and promotes the development of advanced cathode materials with long durability.

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高机械化学稳定性富锂锰基氧化物的相干抑制相构建
一种层状富锂锰基氧化物阴极,包含R3 m (LiTMO2, TM = Mn, Ni, Co)和C2/m (Li2MnO3)纳米畴,利用过渡金属和氧氧化还原产生可观的能量密度。然而,层状富锂氧化物固有的非均相性质和独特的纳米畴氧化还原化学性质将不可避免地导致有害的晶格应变和结构位移,这很难通过传统的掺杂或涂层策略消除,从而导致性能加速衰减。在此,我们在层状结构中加入了一种抑制应变的钙钛矿相,以有效地抑制锂离子不均匀提取过程中的位移和晶格应变。设计的阴极的机械化学稳定性增强,有利于结构的持久性和氧氧化还原的可逆性,从而实现高的初始库仑效率和稳定的循环和电压分布。我们的晶格工程方法减轻了非均质纳米畴之间非均匀反应性引起的应变和位移,促进了具有长寿命的先进正极材料的发展。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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