journal article·2023-01Open access

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

Bin‐Wei Zhang, Liuyue Cao, Cheng Tang, Chunhui Tan, Ningyan Cheng, Wei‐Hong Lai, Yun‐Xiao Wang, Zhen‐Xiang Cheng, Juncai Dong, Yuan Kong, Shi‐Xue Dou, Shenlong Zhao

Advanced Materials· Volume 35· Issue 1

Abstract

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‐MoS2 and Mo1 (S@MoS2‐Mo1/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@MoS2‐Mo1/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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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Thermal Expansion and Ionic Conductivity · Advancements in Battery Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Chemistry and Chemical Engineering Chongqing University Chongqing 400044 P. R. China

Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary Studies Chongqing University Chongqing 400044 P. R. China

Institute for Superconducting and Electronic Materials Australian Institute of Innovative Materials University of Wollongong Innovation Campus, SquiresWay, North Wollongong New South Wales 2500 Australia

The University of Sydney School of Chemical and Biomolecular Engineering Sydney New South Wales 2006 Australia

School of Chemical Engineering The University of Adelaide Adelaide South Australia 5005 Australia

Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 P. R. China

Hefei National Laboratory for Physical Sciences at the Microscale Synergetic Innovation Center of Quantum Information and Quantum Physics University of Science and Technology of China Hefei 230026 P. R. China

Funding

National Natural Science Foundation of China · Fundamental Research Funds for the Central Universities · Australian Research Council

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