Issue 4, 2021

Blocking polysulfides with a Janus Fe3C/N-CNF@RGO electrode via physiochemical confinement and catalytic conversion for high-performance lithium–sulfur batteries

Abstract

Lithium–sulfur batteries (LSBs) have shown great potential for application in high-density energy storage systems. However, the performance of LSBs is severely hindered by the shuttle effect and the sluggish reaction kinetics of lithium polysulfides (LiPSs). Here, a Janus Fe3C/N-CNF@RGO electrode consisting of a 1D Fe3C-decorated N-doped carbon nanofibers (Fe3C/N-CNFs) side and a 2D reduced graphene oxide (RGO) side was applied as a free-standing carrier for the Li2S6 catholyte to improve the overall electrochemical performance of LSBs. The Fe3C/N-CNF layer endows the cathode with strong chemisorption abilities for LiPSs and accelerated the redox kinetics via catalyzing the conversion of LiPSs. The 2D RGO sheets serve as a microscopic physical barrier and further resist the shuttling of LiPSs. Like a hunter's trap, behind the trap lies a net. Moreover, the 3D hierarchical conductive network based on 1D N-CNF and 2D RGO sheets enables fast electron transfer. Based on the synergetic effects of chemical immobilization, catalytic abilities, and a physical barrier in a 3D conductive network, LSBs with optimal Fe3C/N-CNF@RGO electrodes exhibit robust long-term cycling stability (a decay rate of only 0.0089% per cycle at 0.5C for 300 cycles), superior rate capabilities (821.7 mA h g−1 at 2.0C), and stable cycling performance at high sulfur loading (6.29 mg cm−2). This work defines an emerging viewpoint relating to the design of novel sulfur carriers with multiple synergistic effects for application in LSBs.

Graphical abstract: Blocking polysulfides with a Janus Fe3C/N-CNF@RGO electrode via physiochemical confinement and catalytic conversion for high-performance lithium–sulfur batteries

Supplementary files

Article information

Article type
Paper
Submitted
28 Oct 2020
Accepted
13 Dec 2020
First published
15 Dec 2020

J. Mater. Chem. A, 2021,9, 2205-2213

Blocking polysulfides with a Janus Fe3C/N-CNF@RGO electrode via physiochemical confinement and catalytic conversion for high-performance lithium–sulfur batteries

J. Li, H. Zhang, L. Luo, H. Li, J. He, H. Zu, L. Liu, H. Liu, F. Wang and J. Song, J. Mater. Chem. A, 2021, 9, 2205 DOI: 10.1039/D0TA10515E

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