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<p>The development of substrates capable of anchoring single-atom catalysts (SACs) while enabling their dynamic reconfiguration into heteronuclear dual-atom catalysts (DACs) holds considerable promise for electrochemical synthesis, yet remains underexplored. Here we show that electrochemical desulfurization of MoS<sub>2</sub> generates vacancy-rich 1T′ domains, which support high loadings of Cu (7.9 wt%) and Pt (6.7 wt%) SACs that are well-positioned for dynamic sintering to form DACs. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a voltage-driven, reversible transformation between individual Pt/Cu SACs and Cu–Pt DAC configurations during hydrogen evolution reaction potentials. The electric-field-induced Cu–Pt DACs exhibit superior performance in the selective hydrogenation of alkynes compared with their monometallic SAC counterparts. This work underscores vacancy-enriched 1T′-MoS<sub>2</sub> as a versatile platform for high-density SAC deposition, enabling on-demand structural reconfiguration and paving the way for tailored catalyst design in electrosynthesis.</p>

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Electric bias-induced reversible configuration of single and heteronuclear dual-atom catalysts on 1Tʹ-MoS2

  • 期刊论文

  • 发表日期：

    2025年5月19日

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  • Jianhua Wu,
  • Zhongxin Chen,
  • Ke Yang,
  • Xin Zhou,
  • Huizhi Li,
  • Zhiyong Wang,
  • Mengyao Su,
  • Rongrong Zhang,
  • Tie Wang,
  • Qikun Hu,
  • Ning Yan,
  • Cuibo Liu,
  • Bin Zhang,
  • Ming Yang,
  • Shibo Xi,
  • Kian Ping Loh

摘要

The development of substrates capable of anchoring single-atom catalysts (SACs) while enabling their dynamic reconfiguration into heteronuclear dual-atom catalysts (DACs) holds considerable promise for electrochemical synthesis, yet remains underexplored. Here we show that electrochemical desulfurization of MoS2 generates vacancy-rich 1T′ domains, which support high loadings of Cu (7.9 wt%) and Pt (6.7 wt%) SACs that are well-positioned for dynamic sintering to form DACs. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a voltage-driven, reversible transformation between individual Pt/Cu SACs and Cu–Pt DAC configurations during hydrogen evolution reaction potentials. The electric-field-induced Cu–Pt DACs exhibit superior performance in the selective hydrogenation of alkynes compared with their monometallic SAC counterparts. This work underscores vacancy-enriched 1T′-MoS2 as a versatile platform for high-density SAC deposition, enabling on-demand structural reconfiguration and paving the way for tailored catalyst design in electrosynthesis.