Role of Substitution Elements in Enhancing the Structural Stability of Li-Rich Layered Cathodes

Element doping/substitution has been recognized as an effective strategy to enhance the structural stability of layered cathodes. However, abundant substitution studies not only lack a clear identification of the substitution sites in the material lattice, but the rigid interpretation of the transition metal (TM)-O covalent theory is also not sufficiently convincing, resulting in the doping/substitution proposals being dragged into design blindness. In this work, taking Li1.2Ni0.2Mn0.6O2 as a prototype, the intense correlation between the "disordered degree" (Li/Ni mixing) and interface-structure stability (e.g., TM-O environment, slab/lattice, and Li+ reversibility) is revealed. Specifically, the degree of disorder induced by the Mg/Ti substitution extends in the opposite direction, conducive to sharp differences in the stability of TM-O, Li+ diffusion, and anion redox reversibility, delivering fairly distinct electrochemical performance. Based on the established paradigm of systematic characterization/analysis, the "degree of disorder" has been shown to be a powerful indicator of material modification by element substitution/doping.

Medienart:

E-Artikel

Erscheinungsjahr:

2023

Erschienen:

2023

Enthalten in:

Zur Gesamtaufnahme - year:2023

Enthalten in:

Journal of the American Chemical Society - (2023) vom: 07. Apr.

Sprache:

Englisch

Beteiligte Personen:

Zhang, Baodan [VerfasserIn]
Zhang, Yiming [VerfasserIn]
Wang, Xiaotong [VerfasserIn]
Liu, Hui [VerfasserIn]
Yan, Yawen [VerfasserIn]
Zhou, Shiyuan [VerfasserIn]
Tang, Yonglin [VerfasserIn]
Zeng, Guifan [VerfasserIn]
Wu, Xiaohong [VerfasserIn]
Liao, Hong-Gang [VerfasserIn]
Qiu, Yongfu [VerfasserIn]
Huang, Huan [VerfasserIn]
Zheng, Lirong [VerfasserIn]
Xu, Juping [VerfasserIn]
Yin, Wen [VerfasserIn]
Huang, Zhongyuan [VerfasserIn]
Xiao, Yinguo [VerfasserIn]
Xie, Qingshui [VerfasserIn]
Peng, Dong-Liang [VerfasserIn]
Li, Chao [VerfasserIn]
Qiao, Yu [VerfasserIn]
Sun, Shi-Gang [VerfasserIn]

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Journal Article

Anmerkungen:

Date Revised 08.04.2023

published: Print-Electronic

Citation Status Publisher

doi:

10.1021/jacs.3c01999

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM355339889