Atomically dispersed Fe-N5 coordination structure anchored in defective g-C3N4 as oversaturated asymmetric single-atom catalysts for accelerating redox kinetics in Li-S batteries

doi:10.1016/j.jmst.2024.04.068

Abstract

Abstract: Lithium-sulfur (Li-S) batteries are regarded as the most formidable competitor to lithium-ion batteries due to their superior theoretical capacity. However, the negative impact of soluble lithium polysulfide (LiPSs) and slow redox reaction kinetics seriously hamper the commercialization of Li-S batteries. In this study, a defect-rich single-atom catalyst with an oversaturated asymmetric Fe-N₅ coordination structure anchored in defective g-C₃N₄ (C₃N₄-Fe@rGO) is designed via an absorption-pyrolysis strategy. The two-dimensional (2D) conducting C₃N₄@graphene structure with abundant defect sites accelerates the transfer and transportation of lithium ions and electrons. The oversaturated asymmetric Fe-N₅ coordination structure effectively improves the adsorbility of LiPSs and accelerates the redox kinetics of sulfur species. Hence, the Li-S cell with a C₃N₄-Fe@rGO modified separator reveals a high initial capacity (1197.1 mAh g^-1 at 0.2 C) and a low capacity decay rate (0.037 % per cycle after 900 cycles at 1 C). Even at high sulfur loading and extreme temperatures of 0 °C, it also shows good cycling performance. This work creates ideas for synthesizing oversaturated single-atom coordination environments and an efficient route to the practical realization of the Li-S batteries.

Key words: Defective, Oversaturated asymmetric, Single-atom Fe catalyst, Sulfur conversion kinetics, Lithium-sulfur batteries

Jun Wang, Jinxin Wang, Yongzheng Zhang, Cheng Ma, Jitong Wang, Wenming Qiao, Licheng Ling. Atomically dispersed Fe-N₅ coordination structure anchored in defective g-C₃N₄ as oversaturated asymmetric single-atom catalysts for accelerating redox kinetics in Li-S batteries[J]. J. Mater. Sci. Technol., 2025, 209: 230-239.

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Atomically dispersed Fe-N₅ coordination structure anchored in defective g-C₃N₄ as oversaturated asymmetric single-atom catalysts for accelerating redox kinetics in Li-S batteries

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