Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries

Fu, Fang; Liu, Xiang; Fu, Xiaoguang; Chen, Hongwei; Huang, Ling; Fan, Jingjing; Le, Jiabo; Wang, Qiuxiang; Yang, Weihua; Ren, Yang; Amine, Khalil; Sun, Shi-Gang; Xu, Gui-Liang

doi:10.1038/s41467-022-30113-0

Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries

Journal Article · Fri May 20 00:00:00 EDT 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-30113-0· OSTI ID:1869037

Fu, Fang; Liu, Xiang; Fu, Xiaoguang; ; Huang, Ling; Fan, Jingjing; Le, Jiabo; Wang, Qiuxiang; Yang, Weihua; Ren, Yang; ; Sun, Shi-Gang;

Abstract

P2-type sodium manganese-rich layered oxides are promising cathode candidates for sodium-based batteries because of their appealing cost-effective and capacity features. However, the structural distortion and cationic rearrangement induced by irreversible phase transition and anionic redox reaction at high cell voltage (i.e., >4.0 V) cause sluggish Na-ion kinetics and severe capacity decay. To circumvent these issues, here, we report a strategy to develop P2-type layered cathodes via configurational entropy and ion-diffusion structural tuning. In situ synchrotron X-ray diffraction combined with electrochemical kinetic tests and microstructural characterizations reveal that the entropy-tuned Na _0.62 Mn _0.67 Ni _0.23 Cu _0.05 Mg _0.07 Ti _0.01 O ₂ (CuMgTi-571) cathode possesses more {010} active facet, improved structural and thermal stability and faster anionic redox kinetics compared to Na _0.62 Mn _0.67 Ni _0.37 O ₂ . When tested in combination with a Na metal anode and a non-aqueous NaClO ₄ -based electrolyte solution in coin cell configuration, the CuMgTi-571-based positive electrode enables an 87% capacity retention after 500 cycles at 120 mA g ⁻¹ and about 75% capacity retention after 2000 cycles at 1.2 A g ⁻¹ .

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Huaqiao University; National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); Natural Science Foundation of Fujian Province; USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1869037

Alternate ID(s):: OSTI ID: 1962330

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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