Enhancing the backbone regularity of sulfurized polyacrylonitrile for long-life Li-SPAN batteries

Abstract

The intrinsic solid–solid reactions of sulfurized polyacrylonitrile (SPAN) cathode materials present a compelling solution to tackle the serious issue of “shuttle effect” in lithium–sulfur batteries. However, the intrinsic sluggish kinetics of the SPAN cathode poses challenges to the practical application of Li-SPAN batteries, particularly under high current density. Herein, an innovative SPAN cathode material was designed to overcome the inherent kinetic limitations via a two-step strategy, including controllable pre-cyclization and stabilized vulcanization. The cyclization degree of PAN is ingeniously controlled at relatively low temperatures through oxygen-mediated pre-cyclization, which is characterized by low activation energy, slow reaction rate and limited reaction extent. The vulcanization of the as-prepared PAN leads to enhanced stability and reduced production of defective structures while sufficiently preserving the C–H bonds as the active sites for vulcanization, resulting in an air200-SPAN material with decreased defects and a highly regular backbone structure, which exhibits improved electronic conductivity and ionic diffusion. As a result, the Li-SPAN battery with the air200-SPAN cathode material exhibited superior cycling stability at a challenging 3C (1C = 600 mA h g−1) current density over 1400 cycles, with a retained capacity of 427 mA h g−1 (based on the composite) and an ultra-low capacity fading rate of 0.01% per cycle, demonstrating superior cycling stability. This work has illustrated its potential to address the critical challenges while offering valuable insights toward the realization of high-performance lithium–sulfur batteries.

Graphical abstract: Enhancing the backbone regularity of sulfurized polyacrylonitrile for long-life Li-SPAN batteries

Supplementary files

Article information

Article type
Paper
Submitted
09 3月 2025
Accepted
12 5月 2025
First published
14 5月 2025

J. Mater. Chem. A, 2025, Advance Article

Enhancing the backbone regularity of sulfurized polyacrylonitrile for long-life Li-SPAN batteries

J. Wang, Z. Du, G. Lv, X. Zhao, C. Li, X. Chen and Y. Huang, J. Mater. Chem. A, 2025, Advance Article , DOI: 10.1039/D5TA01918D

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