材料科学
硫黄
阴极
石墨烯
X射线光电子能谱
储能
密度泛函理论
化学工程
纳米技术
化学
物理化学
冶金
计算化学
功率(物理)
工程类
物理
量子力学
作者
Binwei Zhang,Liuyue Cao,Cheng Tang,Chunhui Tan,Ningyan Cheng,Wei‐Hong Lai,Yunxiao Wang,Zhenxiang Cheng,Juncai Dong,Yuan Kong,Shixue Dou,Shenlong Zhao
标识
DOI:10.1002/adma.202206828
摘要
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 2 and Mo 1 (S@MoS 2 ‐Mo 1 /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 2 ‐Mo 1 /SGF display unprecedented cyclic stability with a high initial capacity of 1017 mAh g −1 at 0.1 A g −1 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.
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