Issue 20, 2024

Atom-dominated relay catalysis of high-entropy MXene promotes cascade polysulfide conversion for lithium–sulfur batteries

Abstract

To address the challenges in Li–S batteries, i.e. the shuttle effect and lithium dendrite formation, a high-entropy MXene (HE-MXene) of TiVNbMoC3 with four size-compatible transition metal elements uniformly dispersed in its M-layer is designed as sulfur host and separator modification layer. Through theoretical analysis and experimental investigations, the synergistic engineering of the multi-active centers within the HE-MXene is revealed, which provides high configuration compatibility with lithium polysulfides and optimizes the d-band center. Furthermore, the HE-MXene delivers an atom-dominated relay catalysis effect of Ti, V, Nb and Mo sites throughout the ordered multistep sulfur redox reactions, providing new opportunities for enabling a cascade of trapping-catalysis-conversion towards polysulfides and continuously mitigating the shuttle effect in Li–S chemistry. Moreover, the homogeneous electric field distribution and resilient lattice configuration are facilitated by the HE-MXene on the separator, promoting uniform lithium nucleation and deposition on lithium anode. Leveraging these unique properties, Li–S batteries incorporating the HE-MXene demonstrate a high areal capacity of 4.92 mA h cm−2 at 0.2C after 100 cycles. This study not only introduces the HE-MXene as a solution for shuttle-free sulfur cathodes and dendrite-free lithium anodes, but also provides valuable insights for the rational design of advanced electrocatalysts at the atomic level.

Graphical abstract: Atom-dominated relay catalysis of high-entropy MXene promotes cascade polysulfide conversion for lithium–sulfur batteries

Supplementary files

Article information

Article type
Paper
Submitted
30 Jul 2024
Accepted
06 Sep 2024
First published
10 Sep 2024

Energy Environ. Sci., 2024,17, 7735-7748

Atom-dominated relay catalysis of high-entropy MXene promotes cascade polysulfide conversion for lithium–sulfur batteries

M. Xu, Q. Zhu, Y. Li, Y. Gao, N. Sun and B. Xu, Energy Environ. Sci., 2024, 17, 7735 DOI: 10.1039/D4EE03402C

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