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<p>Atomically dispersed single-atom catalysts (SACs) supported on graphene provide a ladder of opportunity for achieving the electrocatalytic CO<sub>2</sub> reduction to value-added chemicals, where the efficient combinations of active sites and coordination environments are a powerful approach to optimize both activity and selectivity. Nevertheless, the understanding of the underlying mechanism about how the catalytic performance varies via active sites and coordination environments is very limited. Herein, we successfully constructed the activity trend of SACs with different coordination environments (MX<sub><i>n</i></sub>Y<sub>4−<i>n</i></sub> X, Y = N, S, P, and M = 19 transition metals) for CO<sub>2</sub> reduction to CH<sub>4</sub>, using easily obtainable parameters. Based on the entire reaction free energy over 110 stable SACs, the binding strength of *OCHO intermediate (Δ<i>E</i>*<sub>OCHO</sub>) is identified as an initial activity indicator towards CO<sub>2</sub> reduction to CH<sub>4</sub>. With the help of multi-task symbolic regression, a simple active descriptor consisting of intrinsic properties (valence-electron number and electronegativity of metal atoms and coordination atoms) is further constructed, which can well describe the variation of Δ<i>E</i><sub>*OCHO</sub> and the onset potential for CH<sub>4</sub>. Importantly, this active descriptor enables rapid evaluation on the activity of SACs without DFT computations. This work is instructive for the rational design of other CO<sub>2</sub> electrocatalysts and establishing more multiplex descriptors through decoupling the factors and handling them separately.</p>

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Structure-activity relation of single-atom electrocatalysts for CO2 reduction to CH4

  • 期刊论文

  • 发表日期：

    2025年7月2日

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  • Changyan Zhu,
  • Mengxue Wang,
  • Ao Yang,
  • Xiaohui Yao,
  • Guangshan Zhu,
  • Chongyi Ling,
  • Zhongmin Su,
  • Min Zhang

摘要

Atomically dispersed single-atom catalysts (SACs) supported on graphene provide a ladder of opportunity for achieving the electrocatalytic CO2 reduction to value-added chemicals, where the efficient combinations of active sites and coordination environments are a powerful approach to optimize both activity and selectivity. Nevertheless, the understanding of the underlying mechanism about how the catalytic performance varies via active sites and coordination environments is very limited. Herein, we successfully constructed the activity trend of SACs with different coordination environments (MXnY4−n X, Y = N, S, P, and M = 19 transition metals) for CO2 reduction to CH4, using easily obtainable parameters. Based on the entire reaction free energy over 110 stable SACs, the binding strength of *OCHO intermediate (ΔE*OCHO) is identified as an initial activity indicator towards CO2 reduction to CH4. With the help of multi-task symbolic regression, a simple active descriptor consisting of intrinsic properties (valence-electron number and electronegativity of metal atoms and coordination atoms) is further constructed, which can well describe the variation of ΔE*OCHO and the onset potential for CH4. Importantly, this active descriptor enables rapid evaluation on the activity of SACs without DFT computations. This work is instructive for the rational design of other CO2 electrocatalysts and establishing more multiplex descriptors through decoupling the factors and handling them separately.