Atomically Dispersed Dual-Site Cathode with a Record High Sulfur Mass Loading for High-Performance Room-Temperature Sodium-Sulfur Batteries.

Zhang, Bin-Wei; Cao, Liuyue; Tang, Cheng; Tan, Chunhui; Cheng, Ningyan; Lai, Wei-Hong; Wang, Yun-Xiao; Cheng, Zhen-Xiang et al. · Adv Mater · 2023

basic_science · Level V

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Abstract

Room-temperature sodium-sulfur (RT-Na/S) batteries possess high potential for grid-scale stationary energy storage due to their low cost and high energy density. However, the issues arising from the low S mass loading and poor cycling stability caused by the shuttle effect of polysulfides seriously limit their operating capacity and cycling capability. Herein, sulfur-doped graphene frameworks supporting atomically dispersed 2H-MoS<sub>2</sub> and Mo<sub>1</sub> (S@MoS<sub>2</sub> -Mo<sub>1</sub> /SGF) with a record high sulfur mass loading of 80.9 wt.% are synthesized as an integrated dual active sites cathode for RT-Na/S batteries. Impressively, the as-prepared S@MoS<sub>2</sub> -Mo<sub>1</sub> /SGF display unprecedented cyclic stability with a high initial capacity of 1017 mAh g<sup>-1</sup> at 0.1 A g<sup>-1</sup> and a low-capacity fading rate of 0.05% per cycle over 1000 cycles. Experimental and computational results including X-ray absorption spectroscopy, in situ synchrotron X-ray diffraction and density-functional theory calculations reveal that atomic-level Mo in this integrated dual-active-site forms a delocalized electron system, which could improve the reactivity of sulfur and reaction reversibility of S and Na, greatly alleviating the shuttle effect. The findings not only provide an effective strategy to fabricate high-performance dual-site cathodes, but also deepen the understanding of their enhancement mechanisms at an atomic level.