Engineering of single atomic Fe-N4 sites on hollow carbon cages to achieve highly reversible MoS2 anodes for Li-ion batteries

Jing Ren; Hao Guo; Zihan Wang; Guoqiang Ling; Jianqiang Han; Rui-Peng Ren; Yongkang-Lv

doi:10.1016/j.jcis.2024.03.023

Engineering of single atomic Fe-N₄ sites on hollow carbon cages to achieve highly reversible MoS₂ anodes for Li-ion batteries

J Colloid Interface Sci. 2024 Jun 15:664:45-52. doi: 10.1016/j.jcis.2024.03.023. Epub 2024 Mar 6.

Authors

Jing Ren¹, Hao Guo², Zihan Wang², Guoqiang Ling¹, Jianqiang Han³, Rui-Peng Ren⁴, Yongkang-Lv⁵

Affiliations

¹ College of Chemistry, Taiyuan University of Technology, Taiyuan 030024, China.
² State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China.
³ School of Semiconductor and Physics, North University of China, Taiyuan 030051, China. Electronic address: hanjianqiang@nuc.edu.cn.
⁴ State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China; Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030017, China. Electronic address: renruipeng@tyut.edu.cn.
⁵ State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China; Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030017, China.

PMID: 38458054
DOI: 10.1016/j.jcis.2024.03.023

Abstract

Although the single atom electrocatalysts have been demonstrated as efficient catalysts for promoting Li₂S/Na₂S formation and decomposition in Li-S/Na-S batteries, the functional morphological and structural engineering capable of exposing more active sites is regarded as an essential factor to further enhance the catalytic activity. Here, we have synthesized a single atomically dispersed Fe sites embedded within hollow nitrogen doped carbon cages (Fe-N-HCN) using Fe₃O₄ spheres as an oxidant and sacrificial template, which is used as a high-efficiency catalyst for boosting the reversible capacity of MoS₂ anode in lithium-ion batteries (LIBs). As expected, the electrochemical reaction of MoS₂/Fe-N-HCN anode exhibits higher reversibility than pure MoS₂ electrodes. Moreover, density functional theory is also employed to reveal that Fe-N-HCN can be effectively adsorbed and catalyze the rapid decomposition of Li₂S. The hollow carbon cage structure can facilitate the exposure of the active Fe-N₄ sites and favor the mass transfer during the electrochemical reactions, thus the synergistic effect of the Fe-N₄ site and the hollow carbon cage structure together improve the catalytic activity for the conversion reaction of MoS₂ anode.

Keywords: Anode; Lithium-ion battery; MoS(2); Reversible conversion; Single-atom catalysts.