Magnetopyrite Fe1-xS modified with N/S-doped carbon as a synergistic electrocatalyst for lithium-sulfur batteries

Ziwei Zhao; Haoyun Dou; Xuanpan Xu; Rongjie Zhe; Qingye Zhao; Lingxia Zheng; Xinjun Bao; Ting Zhu; Hong-En Wang

doi:10.1016/j.jcis.2025.01.028

Magnetopyrite Fe_1-xS modified with N/S-doped carbon as a synergistic electrocatalyst for lithium-sulfur batteries

J Colloid Interface Sci. 2025 Jan 6;684(Pt 1):180-191. doi: 10.1016/j.jcis.2025.01.028. Online ahead of print.

Authors

Ziwei Zhao¹, Haoyun Dou¹, Xuanpan Xu¹, Rongjie Zhe¹, Qingye Zhao¹, Lingxia Zheng², Xinjun Bao³, Ting Zhu¹, Hong-En Wang⁴

Affiliations

¹ College of Physics and Electronic Information, Yunnan Normal University, 650500 Kunming, China.
² Department of Applied Chemistry, Petroleum and Chemical Industry Key Laboratory of Organic Electrochemical Synthesis, Zhejiang University of Technology, 310014 Hangzhou, China.
³ School of Textile and Fashion, Hunan Institute of Engineering, 411104 Xiangtan, China. Electronic address: xinjunbCSU@126.com.
⁴ College of Physics and Electronic Information, Yunnan Normal University, 650500 Kunming, China. Electronic address: hongen.wang@ynnu.edu.cn.

PMID: 39793426
DOI: 10.1016/j.jcis.2025.01.028

Abstract

Rational design of effective cathode host materials is an effective way to solve the problems of serious shuttle and slow conversion of polysulfides in lithium-sulfur batteries (LSBs). However, the redox reaction of sulfur differs from conventional "Rocking chair" type batteries and involves a cumbersome phase transition process, so a single-component catalyst cannot consistently and steadily enhance the reaction rate throughout the redox process. In this work, a hybrid composed of magnetopyrite Fe_1-xS catalyst-modified with N/S-doped porous carbon spheres (Fe_1-xS@NSC) is proposed as a novel sulfur host to synergistically promote the adsorption and redox catalysis conversion of polysulfides. In this hybrid, the NSC skeleton provides excellent electrical conductivity and abundant adsorption sites for the physical immobilization of polysulfides; the magnetopyrite Fe_1-xS nanoparticles promote the fast conversion reaction from Li₂S₂ to Li₂S, affording strong adsorption and catalytic conversion. The optimal LSB with Fe_1-xS@NSC manifests a high initial capacity of 971 mAh g^-1 at 0.2 C (1 C = 1675 mAh g^-1) and a retention rate of up to 75 % after 100 cycles. This work can provide a new approach for rationalizing the novel transition metal sulfide/porous carbon-based composite hosts with efficient lithium polysulfides (LiPSs) adsorption and catalytic conversion in high-performance lithium-sulfur batteries.

Keywords: Electrocatalysis; Lithium-sulfur batteries; Magnetopyrite phase; Metal sulfides; Nitrogen and sulfur co-doped carbon; Shuttle effect.