Issue 13, 2022

Na2.4Al0.4Mn2.6O7 anionic redox cathode material for sodium-ion batteries – a combined experimental and theoretical approach to elucidate its charge storage mechanism

Abstract

Here we report the synthesis via ceramic methods of the high-performance Mn-rich Na2.4Al0.4Mn2.6O7 oxygen-redox cathode material for Na-ion batteries, which we use as a testbed material to study the effects of Al substitution and subsequent Na excess in the high-capacity, anionic redox-based cathode material, Na2Mn3O7. The material shows a stable electrochemical performance, with a specific capacity of 215 mA h g−1 in the 1.5–4.7 V voltage range at C/20 and a capacity retention of 90% after 40 cycles. Using a combination of electrochemical and structural analysis together with hybrid density functional theory calculations we explain the behaviour of this material with changes in Mn/anionic redox reactions and associated O2 release reactions occurring during electrochemical cycling (Na+ ion insertion/extraction), and compare these findings to Na2Mn3O7. We expect that these results will advance understanding of the effect of dopants in Mn-rich cathode materials with oxygen redox activity to pave their way towards high-performance sodium-ion batteries.

Graphical abstract: Na2.4Al0.4Mn2.6O7 anionic redox cathode material for sodium-ion batteries – a combined experimental and theoretical approach to elucidate its charge storage mechanism

Supplementary files

Article information

Article type
Paper
Submitted
17 6 2021
Accepted
16 12 2021
First published
16 12 2021
This article is Open Access
Creative Commons BY license

J. Mater. Chem. A, 2022,10, 7341-7356

Na2.4Al0.4Mn2.6O7 anionic redox cathode material for sodium-ion batteries – a combined experimental and theoretical approach to elucidate its charge storage mechanism

C. Soares, B. Silván, Y. Choi, V. Celorrio, V. R. Seymour, G. Cibin, J. M. Griffin, D. O. Scanlon and N. Tapia-Ruiz, J. Mater. Chem. A, 2022, 10, 7341 DOI: 10.1039/D1TA05137G

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