Issue 27, 2024

Theoretical insights into single-atom catalysts for improved charging and discharging kinetics of Na–S and Na–Se batteries

Abstract

Dissolution of poly-sulfide/selenides (p-S/Ses) intermediates into electrolytes, commonly known as the shuttle effect, has posed a significant challenge in the development of more efficient and reliable Na–S/Se batteries. Single-atom catalysts (SACs) play a crucial role in mitigating the shuttling of Na–pS/Ses and in promoting Na2S/Se redox processes at the cathode. In this work, single transition metal atoms Co, Fe, Ir, Ni, Pd, Pt, and Rh supported in nitrogen-deficient graphitic carbon nitride (rg-C3N4) are investigated to explore the charging and discharging kinetics of Na–S and Na–Se batteries using Density Functional Theory calculations. We find that SAs adsorbed on reduced g-C3N4 monolayers are substantially more effective in trapping higher-order Na2Xn than pristine g-C3N4 surfaces. Moreover, our ab initio molecular dynamics calculations indicate that the structure of X8 (X = S, Se) remains almost intact when adsorbed on Fe, Co, Ir, Ni, Pt, and Rh SACs, suggesting that there is no significant S or Se poisoning in these cases. Additionally, SACs reduce the free energies of the rate-determining step during discharge and present a lower decomposition barrier of Na2X during charging of Na–X electrode. The underlying mechanisms behind this fast kinetics are thoroughly examined using charge transfer, bonding strength, and d-band center analysis. Our work demonstrates an effective strategy for designing single-atom catalysts and offers solutions to the performance constraints caused by the shuttle effect in sodium–sulfur and sodium–selenium batteries.

Graphical abstract: Theoretical insights into single-atom catalysts for improved charging and discharging kinetics of Na–S and Na–Se batteries

Supplementary files

Article information

Article type
Paper
Submitted
15 mar 2024
Accepted
13 iyn 2024
First published
17 iyn 2024

Nanoscale, 2024,16, 12982-12991

Theoretical insights into single-atom catalysts for improved charging and discharging kinetics of Na–S and Na–Se batteries

M. Jakhar, V. Barone and Y. Ding, Nanoscale, 2024, 16, 12982 DOI: 10.1039/D4NR01134A

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