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<p>Aqueous redox flow batteries (RFBs) incorporating polysulfide/iodide chemistries have received considerable attention due to their safety, high scalability, and cost-effectiveness. However, the sluggish redox kinetics restricted their output energy efficiency and power density. Here we designed a defective MoS<sub>2</sub> nanosheets supported Co single-atom catalyst that accelerated the transformation of S<sup>2−</sup>/S<sub><i>x</i></sub><sup>2−</sup> and I<sup>−</sup>/I<sub>3</sub><sup>−</sup> redox couples, hence endow the derived polysulfide–iodide RFB with an initial energy efficiency (EE) of 87.9% and an overpotential of 113 mV with an average EE 80.4% at 20 mA cm<sup>−2</sup> and 50% state-of-charge for 50 cycles, and a maximal power density of 95.7 mW cm<sup>−2</sup> for an extended cycling life exceeding 850 cycles at 10 mA cm<sup>−2</sup> and 10% state-of-charge. In situ experimental and theoretical analyses elucidate that Co single atoms induce the generation of abundant sulfur vacancies in MoS<sub>2</sub> via a phase transition process, which synergistically contributed to the enhanced adsorption of reactants and key reaction intermediates and improved charge transfer, resulting in the enhanced RFB performance.</p>

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Synergy of single atoms and sulfur vacancies for advanced polysulfide–iodide redox flow battery

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月25日

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  • Zhigui Wang,
  • Guolong Lu,
  • Tianran Wei,
  • Ge Meng,
  • Haoxiang Cai,
  • Yanhong Feng,
  • Ke Chu,
  • Jun Luo,
  • Guangzhi Hu,
  • Dingsheng Wang,
  • Xijun Liu

摘要

Aqueous redox flow batteries (RFBs) incorporating polysulfide/iodide chemistries have received considerable attention due to their safety, high scalability, and cost-effectiveness. However, the sluggish redox kinetics restricted their output energy efficiency and power density. Here we designed a defective MoS2 nanosheets supported Co single-atom catalyst that accelerated the transformation of S2−/Sx2− and I−/I3− redox couples, hence endow the derived polysulfide–iodide RFB with an initial energy efficiency (EE) of 87.9% and an overpotential of 113 mV with an average EE 80.4% at 20 mA cm−2 and 50% state-of-charge for 50 cycles, and a maximal power density of 95.7 mW cm−2 for an extended cycling life exceeding 850 cycles at 10 mA cm−2 and 10% state-of-charge. In situ experimental and theoretical analyses elucidate that Co single atoms induce the generation of abundant sulfur vacancies in MoS2 via a phase transition process, which synergistically contributed to the enhanced adsorption of reactants and key reaction intermediates and improved charge transfer, resulting in the enhanced RFB performance.