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<p>Single-atom catalysts (SACs), constructed by immobilizing transition-metal (TM) atoms on two-dimensional (2D) supports, have attracted widespread interest due to their exceptional atomic efficiency and tunable coordination environments. Nevertheless, current research predominantly focuses on carbon-based materials, with studies on alternative substrate types remaining relatively limited. Herein, we employ first-principles calculations to systematically assess the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) activities of SACs (TM@SiP<sub>3</sub>), which are constructed by anchoring TM atoms onto a 2D SiP<sub>3</sub> monolayer. Among all the stable configurations, Ni@SiP<sub>3</sub> exhibits outstanding HER activity, characterized by a very low hydrogen adsorption free energy (Δ<i>G</i><sub>H*</sub>) of 0.05&#xa0;eV. Meanwhile, Rh@SiP<sub>3</sub> demonstrates the highest OER activity with an ultralow overpotential (<i>η</i>) of 0.46&#xa0;V, along with an ORR overpotential of 0.71&#xa0;V, identifying it as an excellent bifunctional catalyst. Additionally, Pt@SiP<sub>3</sub> also shows promising bifunctional activity for both HER (Δ<i>G</i><sub>H*</sub> = 0.10&#xa0;eV) and ORR (<i>η</i><sup>ORR</sup> = 0.61&#xa0;V). This study expands the design paradigm for multifunctional electrocatalysts and provides valuable insights into the exploration of SACs based on 2D non-carbon substrates.</p> Graphical Abstract <p></p>

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Computational Screening of Single-Atom Catalysts on Two-dimensional SiP3 Monolayer for HER, OER, and ORR

  • 期刊论文

  • 发表日期：

    2026年4月27日

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  • Deyun Meng,
  • Yanqing Shen,
  • Lingling Lv,
  • Xianghui Meng,
  • Bing Zhang,
  • Dewei Gong,
  • Qing Ai,
  • Yong Shuai,
  • Zhongxiang Zhou

摘要

Single-atom catalysts (SACs), constructed by immobilizing transition-metal (TM) atoms on two-dimensional (2D) supports, have attracted widespread interest due to their exceptional atomic efficiency and tunable coordination environments. Nevertheless, current research predominantly focuses on carbon-based materials, with studies on alternative substrate types remaining relatively limited. Herein, we employ first-principles calculations to systematically assess the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) activities of SACs (TM@SiP3), which are constructed by anchoring TM atoms onto a 2D SiP3 monolayer. Among all the stable configurations, Ni@SiP3 exhibits outstanding HER activity, characterized by a very low hydrogen adsorption free energy (ΔGH*) of 0.05 eV. Meanwhile, Rh@SiP3 demonstrates the highest OER activity with an ultralow overpotential (η) of 0.46 V, along with an ORR overpotential of 0.71 V, identifying it as an excellent bifunctional catalyst. Additionally, Pt@SiP3 also shows promising bifunctional activity for both HER (ΔGH* = 0.10 eV) and ORR (ηORR = 0.61 V). This study expands the design paradigm for multifunctional electrocatalysts and provides valuable insights into the exploration of SACs based on 2D non-carbon substrates.

Graphical Abstract