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Conversion of Co Nanoparticles to CoS in Metal–Organic Framework-Derived Porous Carbon during Cycling Facilitates Na2S Reactivity in a Na–S Battery

  • Ruixian Zhang
    Ruixian Zhang
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
  • Anne Marie Esposito
    Anne Marie Esposito
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
  • Eric S. Thornburg
    Eric S. Thornburg
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
  • Xinyi Chen
    Xinyi Chen
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
    More by Xinyi Chen
  • Xueyong Zhang
    Xueyong Zhang
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
  • Maria A. Philip
    Maria A. Philip
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
  • Alexis Magana
    Alexis Magana
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
  • , and 
  • Andrew A. Gewirth*
    Andrew A. Gewirth
    Department of Chemistry, University of Illinois, Urbana, Illinois 61801, United States
    *Email: [email protected]. Tel.: +1-217-333-8329.
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 26, 29285–29295
Publication Date (Web):June 3, 2020
https://doi.org/10.1021/acsami.0c05370
Copyright © 2020 American Chemical Society
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Abstract

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Room-temperature sodium–sulfur batteries have attracted wide interest due to their high energy density and high natural abundance. Polysulfide dissolution and irreversible Na2S conversion are challenges to achieving high battery performance. Herein, we utilize a metal–organic framework-derived Co-containing nitrogen-doped porous carbon (CoNC) as a catalytic sulfur cathode host. A concentrated sodium electrolyte based on sodium bis(fluorosulfonyl)imide, dimethoxyethane, and bis(2,2,2-trifluoroethyl) ether is used to mitigate polysulfide dissolution. We tune the amount of Co present in the CoNC carbon host by acid washing. Significant improvement in reversible sulfur conversion and capacity retention is observed with a higher Co content in CoNC, with 600 mAh g–1 and 77% capacity retention for CoNC and 261 mAh g–1 and 56% capacity retention for acid-washed CoNC at cycle 50 at 80 mAh g–1. Post-mortem X-ray photoelectron spectroscopy, transmission electron microscopy, and selected area electron diffraction suggest that CoS is formed during cycling in place of Co nanoparticles and CoN4 sites. Raman spectroscopy suggests that CoS exhibits a catalytic effect on the oxidation of Na2S. Our findings provide insights into understanding the role Co-based catalysts play in sulfur batteries.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c05370.

  • VSM data, EIS data, discharge–charge curves, XRD pattern, and cycling data of various samples (PDF)

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Cited By

This article is cited by 3 publications.

  1. Ling Zhao, Feng Qiu, Xiaohua Deng, Yun Huang, Yuntao Li, Chunxia Zhao, Wenhao Ren, Chao Zou, Xing Li, Mingshan Wang, Yuanhua Lin. Novel Sulfur-Containing Polymeric Cathode Material Prepared via an Inverse Vulcanization Method for Advanced Lithium–Sulfur Batteries. ACS Applied Energy Materials 2022, 5 (6) , 7617-7626. https://doi.org/10.1021/acsaem.2c00866
  2. Ye Wang, Xiang Long Huang, Hanwen Liu, Weiling Qiu, Chi Feng, Ce Li, Shaohui Zhang, Hua Kun Liu, Shi Xue Dou, Zhiming M. Wang. Nanostructure Engineering Strategies of Cathode Materials for Room-Temperature Na–S Batteries. ACS Nano 2022, 16 (4) , 5103-5130. https://doi.org/10.1021/acsnano.2c00265
  3. Xue Feng Lu, Yongjin Fang, Deyan Luan, Xiong Wen David Lou. Metal–Organic Frameworks Derived Functional Materials for Electrochemical Energy Storage and Conversion: A Mini Review. Nano Letters 2021, 21 (4) , 1555-1565. https://doi.org/10.1021/acs.nanolett.0c04898

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