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Title: Boosting electrochemical reaction and suppressing phase transition with a high-entropy O3-type layered oxide for sodium-ion batteries

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/d2ta02451a· OSTI ID:1982260
 [1];  [1];  [1];  [2]; ORCiD logo [2];  [2]; ORCiD logo [3];  [2];  [4]
  1. Northeastern University, Shenyang (China)
  2. Northeastern University, Shenyang and Qinhuangdao (China)
  3. Northeastern University at Qinhuangdao (China)
  4. Yangzhou Univ., Jiangsu (China)
+ Show Author Affiliations

Complex phase transitions induced by interlayer slides in layered cathode materials lead to poor cycling stability and rate capability for sodium-ion batteries. Herein, we design and prepare a new six-component high-entropy oxide (HEO) layered cathode O3–Na(Fe0.2Co0.2Ni0.2Ti0.2Sn0.1Li0.1)O2 to enable highly reversible electrochemical reaction and phase-transition behavior. The HEO cathode exhibits good cycling performance (capacity retention of ~81% after 100 cycles at 0.5C) and outstanding rate capability (capacity of ~81 mA h g–1 at 2.0C) due to the higher sodium diffusion coefficient (above 5.75 × 10–11 cm2 s–1) than most reported O3-type cathodes. Moreover, the high-entropy cathode has superior compatibility with the hard carbon anode and delivers a specific capacity of 90.4 mA h g–1 (energy density of ~267.5 W h kg–1). Ex situ X-ray diffraction proves that the high-entropy designing effectively suppresses the intermediate phase change to achieve reversible O3–P3 phase evolution, and in turn stabilizes the layered structure. X-ray absorption spectroscopy and Mössbauer spectrum of 57Fe suggest that Ni2+/Ni3.5+, Co3+/Co3.5+, and part of Fe3+/Fe3.5+ redox reaction contribute the charge compensation. Finally, the enhanced performance can be attributed to the disordered distribution of multi-component transition metals in HEO suppressing the ordering of electric charges and sodium vacancies, thereby inhibiting the interlayer slide and phase transition.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Organization:
USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC); Natural Science Foundation of Hebei Province; Fundamental Research Funds for the Central Universities
Grant/Contract Number:
SC0012704; 52071073; 51902046; 52071085; 51871046; 52171202; 52177208; 51971055; E2020501004; N2123032
OSTI ID:
1982260
Alternate ID(s):
OSTI ID: 1874423
Journal Information:
Journal of Materials Chemistry. A, Vol. 10, Issue 28; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Figures / Tables (7)

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry
Energy &amp; Fuels
Materials science
sodium-ion batteries
layered cathode
high-entropy oxide
phase transition