Soares, C; Silvan, B; Choi, Y-S; Celorrio, V; Cibin, G; Scanlon, DO; Tapia-Ruiz, N; (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. Journal of Materials Chemistry A , 10 (13) pp. 7341-7356. 10.1039/d1ta05137g.

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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 200 mAh g-1 in the 1.5 - 4.7 voltage window at C/20 and 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 in the material during electrochemical cycling (Na 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 real applications in high-performing sodium-ion battery applications.

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