journal article·2023-06-07

Low-Coordinated Zn–N2 Sites as Bidirectional Atomic Catalysis for Room-Temperature Na–S Batteries

Daliang Fang, Shaozhuan Huang, Tingting Xu, Pan Sun, Xue Liang Li, Yew Von Lim, Dong Yan, Yang Shang, Bing-Jian Su, Jenh-Yih Juang, Qi Ge, Hui Ying Yang

ACS Applied Materials & Interfaces· Volume 15· Issue 22
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Abstract

The rational design of advanced catalysts for sodium–sulfur (Na–S) batteries is important but remains challenging due to the limited understanding of sulfur catalytic mechanisms. Here, we propose an efficient sulfur host consisting of atomic low-coordinated Zn–N 2 sites dispersed on N-rich microporous graphene (Zn–N 2 @NG), which realizes state-of-the-art sodium-storage performance with a high sulfur content of 66 wt %, high-rate capability (467 mA h g –1 at 5 A g –1 ), and long cycling stability for 6500 cycles with an ultralow capacity decay rate of 0.0062% per cycle. Ex situ methods combined with theoretical calculations demonstrate the superior bidirectional catalysis of Zn–N 2 sites on sulfur conversion (S 8 ↔ Na 2 S). Furthermore, in situ transmission electron microscopy was applied to visualize the microscopic S redox evolution under the catalysis of Zn–N 2 sites without liquid electrolytes. During the sodiation process, both surface S nanoparticles and S molecules in the mircopores of Zn–N 2 @NG quickly convert into Na 2 S nanograins. During the following desodiation process, only a small part of the above Na 2 S can be oxidized into Na 2 S x . These results reveal that, without liquid electrolytes, Na 2 S is difficult to be decomposed even with the assistance of Zn–N 2 sites. This conclusion emphasizes the critical role of liquid electrolytes in the catalytic oxidation of Na 2 S, which was usually ignored by previous works.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced battery technologies research

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Affiliations

Pillar of Engineering Product Development, Singapore University of Technology and Design, 8 Somapah Road, Singapore 487372, Singapore

Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education, South-Central University for Nationalities, Wuhan, Hubei 430074, China

Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450052, China

NSF’S ChemMatCARS, University of Chicago, Chicago, Illinois 60637, United States

International Joint Laboratory of New Energy Materials and Devices of Henan Province, School of Physics & Electronics, Henan University, Kaifeng 475004, China

Institute of Advanced Battery Materials and Devices, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China

Department of Electrophysics, National Chiao Tung University, 1001 Ta-Hsueh Road, Hsinchu 30010, Taiwan, ROC

Shenzhen Key Laboratory of Biomimetic Robotics and Intelligent Systems, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, China

Funding

Ministry of Education - Singapore · National Natural Science Foundation of China

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