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Built-In Catalysis in Confined Nanoreactors for High-Loading Li–S Batteries

  • Qingping Wu
    Qingping Wu
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    More by Qingping Wu
  • Zhenguo Yao
    Zhenguo Yao
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
    More by Zhenguo Yao
  • Xuejun Zhou
    Xuejun Zhou
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    More by Xuejun Zhou
  • Jun Xu*
    Jun Xu
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    *Email: [email protected]
    More by Jun Xu
  • Fahai Cao
    Fahai Cao
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    More by Fahai Cao
  • , and 
  • Chilin Li*
    Chilin Li
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
    *Email: [email protected]
    More by Chilin Li
Cite this: ACS Nano 2020, 14, 3, 3365–3377
Publication Date (Web):March 2, 2020
https://doi.org/10.1021/acsnano.9b09231
Copyright © 2020 American Chemical Society
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Abstract

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A cathode host with strong sulfur/polysulfide confinement and fast redox kinetics is a challenging demand for high-loading lithium–sulfur batteries. Recently, porous carbon hosts derived from metal–organic frameworks (MOFs) have attracted wide attention due to their unique spatial structure and customizable reaction sites. However, the loading and rate performance of Li–S cells are still restricted by the disordered pore distribution and surface catalysis in these hosts. Here, we propose a concept of built-in catalysis to accelerate lithium polysulfide (LiPSs) conversion in confined nanoreactors, i.e., laterally stacked ordered crevice pores encompassed by MoS2-decorated carbon thin layers. The functions of S-fixability and LiPS catalysis in these mesoporous cavity reactors benefit from the 2D interface contact between ultrathin catalytic MoS2 and conductive C pyrolyzed from Al-MOF. The integrated function of adsorption–catalysis–conversion endows the sulfur-infused [email protected]2 electrode with a high initial capacity of 1240 mAh g–1 at 0.2 C, long life cycle stability of at least 1000 cycles at 2 C, and high rate endurance up to 20 C. This electrode also exhibits commercial potential in view of considerable capacity release and reversibility under high sulfur loading (6 mg cm–2 and ∼80 wt %) and lean electrolyte (E/S ratio of 5 μL mg–1). This study provides a promising design solution of a catalysis–conduction 2D interface in a 3D skeleton for high-loading Li–S batteries.

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