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Fast Oxygen Redox Kinetics Induced by CoO6 Octahedron With π–Interaction in P2–Type Sodium Oxides

Journal Article · · Advanced Functional Materials
 [1];  [2];  [1];  [1];  [1];  [3];  [2];  [1];  [1];  [1]
  1. Shanghai Jiao Tong Univ. (China)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Enhancing the kinetics of lattice oxygen redox (LOR) in P2-type layered sodium oxide cathodes is crucial for the advancement of sodium-ion batteries (SIBs) with superior energy and power densities. Electronic structure regulation stands out as a highly effective approach to address the inherent limitations of P2-type layered oxides with LOR, including sluggish kinetics, phase transitions, voltage hysteresis, and local structural distortion. In this work, a strategy involving the introduction of CoO6 octahedra with π-interaction into Na0.6Li0.1Fe0.3–xCoxMn0.6O2 (x = 0, 0.15, 0.3) cathodes to facilitate Na-ion transport is proposed. Furthermore, the impact of FeO6 octahedra with σ-interaction in P2-type cathodes on electrochemical performance is comprehensively investigated. Through multimodal in-situ and ex-situ characterization techniques, it is revealed that Co–O with π-interaction effectively mitigates P2-OP4 phase transitions by strengthening Na–O, reduces voltage hysteresis, and stabilizes the local structure. Consequently, Na0.6Li0.1Co0.3Mn0.6O2 demonstrates enhanced Na-ion diffusion kinetics, leading to improved rate performance and a reversible capacity of 55 mAh g–1 at 10 C, significantly outperforming cathodes with Fe–O σ-interaction. Moreover, when coupled with hard carbon, the full cell achieves a remarkable energy density of 395 Wh kg–1 (on cathode) at 0.1 C, with a capacity retention of 75% over 100 cycles at 1 C.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Natural Science Foundation of China (NSFC); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704
OSTI ID:
2440520
Alternate ID(s):
OSTI ID: 2434069
Report Number(s):
BNL--226051-2024-JAAM
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 15 Vol. 34; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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