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

Abstract

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 .

Authors:

Fu, Fang; Liu, Xiang; Fu, Xiaoguang; Chen, Hongwei ;

• Search DOE PAGES for author "Chen, Hongwei"
• Search DOE PAGES for ORCID "0000-0002-1401-9680"

Huang, Ling; Fan, Jingjing; Le, Jiabo; Wang, Qiuxiang; Yang, Weihua; Ren, Yang; Amine, Khalil ;

• Search DOE PAGES for author "Amine, Khalil"
• Search DOE PAGES for ORCID "0000-0001-9206-3719"

Sun, Shi-Gang; Xu, Gui-Liang

• Search DOE PAGES for author "Xu, Gui-Liang"
• Search DOE PAGES for ORCID "0000-0001-9969-883X"

Publication Date:

Fri May 20 00:00:00 EDT 2022

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:

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

OSTI Identifier:

1869037

Alternate Identifier(s):

OSTI ID: 1962330

Grant/Contract Number:  

AC02-06CH11357; 21805100; 2016YFB0100202; 2019J05091; 2019J06018; ZQN-PY606

Resource Type:

Published Article

Journal Name:

Nature Communications

Additional Journal Information:

Journal Name: Nature Communications Journal Volume: 13 Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:

Nature Publishing Group

Country of Publication:

United Kingdom

Language:

English

Subject:

25 ENERGY STORAGE; batteries; inorganic chemistry; microscopy