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<p>Carbon-supported single-atom catalysts (C-SACs) have been demonstrated as a strategy to promote the reversible conversion reaction of metal sulfide anodes in sodium-ion batteries (SIBs). However, the design principle of promising C-SACs remains lacking for obtaining highly reversible metal sulfide anodes. We designed a phosphorus-doped carbon-supported single-atom Mn catalyst (PC-SAMn) with an asymmetrical dual active center. The sulfiphilic Mn and sodiophilic P active centers adsorb discharged Na<sub>2</sub>S through Mn–S d-p and P–Na s-p orbital hybridizations. The asymmetrical dual active center induced the asymmetrical adsorption configuration of Na<sub>2</sub>S, which efficiently weakened Na–S bond strength and facilitated the decomposition of Na<sub>2</sub>S during charging. As a result, the designed catalyst enables typical MoS<sub>2</sub> with a record-high compositional reversible degree of 89.61% and a low capacity decay ratio of only 0.18% per 100 cycles during 2000 cycles. The research establishes the “orbital hybridization-molecular structure-catalytic activity” relationship for guiding the design of highly reversible conversion-type materials.</p>

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Regulating the orbital hybridization to induce asymmetrical catalysis for efficient reversible sodium conversion storage

  • 期刊论文

  • 发表日期：

    2025年7月2日

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  • Zijia Qi,
  • Kai Cui,
  • Simi Sui,
  • Yuxuan Wang,
  • Haonan Xie,
  • Guangxuan Wu,
  • Yihao Cheng,
  • Enzuo Liu,
  • Fang He,
  • Chunnian He,
  • Tianshuai Wang,
  • Biao Chen,
  • Naiqin Zhao

摘要

Carbon-supported single-atom catalysts (C-SACs) have been demonstrated as a strategy to promote the reversible conversion reaction of metal sulfide anodes in sodium-ion batteries (SIBs). However, the design principle of promising C-SACs remains lacking for obtaining highly reversible metal sulfide anodes. We designed a phosphorus-doped carbon-supported single-atom Mn catalyst (PC-SAMn) with an asymmetrical dual active center. The sulfiphilic Mn and sodiophilic P active centers adsorb discharged Na2S through Mn–S d-p and P–Na s-p orbital hybridizations. The asymmetrical dual active center induced the asymmetrical adsorption configuration of Na2S, which efficiently weakened Na–S bond strength and facilitated the decomposition of Na2S during charging. As a result, the designed catalyst enables typical MoS2 with a record-high compositional reversible degree of 89.61% and a low capacity decay ratio of only 0.18% per 100 cycles during 2000 cycles. The research establishes the “orbital hybridization-molecular structure-catalytic activity” relationship for guiding the design of highly reversible conversion-type materials.