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<p>Single-atom catalysts (SACs) are promising for hydrogen evolution due to their maximal atomic utilization and discrete energy levels. Modulating metal-support interactions is key to tailoring their activity and stability, yet achieving precise control and mechanistic insight remains challenging and controversial. Here, we construct a rhodium single-atom catalyst model system, with Rh atoms anchored on a series of MoS<sub>x</sub>Se<sub>2-x</sub> supports (Rh<sub>SA</sub>-MoS<sub>x</sub>Se<sub>2-x</sub>, 0 ≤ x ≤ 2), enabling gradient modulation of metal-support frontier orbital interactions through systematic tuning the anion composition. The elevated lowest unoccupied molecular orbital (LUMO) of MoS<sub>x</sub>Se<sub>2-x</sub> support narrows the energy gap with the highest occupied molecular orbital (HOMO) of Rh atoms, strengthening metal-support orbital hybridization to enhance stability and further amending the LUMO of Rh atoms to optimize both the hydroxide and hydrogen adsorption for high activity. The apex Rh<sub>SA</sub>-MoSSe catalyst, with optimal HOMO-LUMO hybridization, achieves favorable hydrogen evolution reaction activity and stability simultaneously. This work offers fundamental insights into the metal-support frontier orbital interaction in SACs and establishes a rational design framework for high activity and stability electrocatalysis.</p>

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Frontier-orbital modulation of rhodium single-atom catalysts for enhanced hydrogen evolution

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月18日

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  • Rouna Jia,
  • Zongyan Liu,
  • Yang Wang,
  • Jingyang Zhao,
  • Zhong Huang,
  • Wen Yue,
  • Haozhi Wang,
  • Kaiping Yu,
  • Mingxin Huang,
  • Yida Deng

摘要

Single-atom catalysts (SACs) are promising for hydrogen evolution due to their maximal atomic utilization and discrete energy levels. Modulating metal-support interactions is key to tailoring their activity and stability, yet achieving precise control and mechanistic insight remains challenging and controversial. Here, we construct a rhodium single-atom catalyst model system, with Rh atoms anchored on a series of MoSxSe2-x supports (RhSA-MoSxSe2-x, 0 ≤ x ≤ 2), enabling gradient modulation of metal-support frontier orbital interactions through systematic tuning the anion composition. The elevated lowest unoccupied molecular orbital (LUMO) of MoSxSe2-x support narrows the energy gap with the highest occupied molecular orbital (HOMO) of Rh atoms, strengthening metal-support orbital hybridization to enhance stability and further amending the LUMO of Rh atoms to optimize both the hydroxide and hydrogen adsorption for high activity. The apex RhSA-MoSSe catalyst, with optimal HOMO-LUMO hybridization, achieves favorable hydrogen evolution reaction activity and stability simultaneously. This work offers fundamental insights into the metal-support frontier orbital interaction in SACs and establishes a rational design framework for high activity and stability electrocatalysis.