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<p>Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to CO using SAC offers a promising approach for CO<sub>2</sub> utilization, but achieving facile CO<sub>2</sub> adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO<sub>2</sub>RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h<sup>−</sup><sup>1</sup> at 500 mA cm<sup>−</sup><sup>2</sup>. Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO<sub>2</sub> conversion efficiency are obtained at 200 mA cm<sup>−</sup><sup>2</sup> with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO<sub>2</sub>-to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts.</p>

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Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月27日

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  • Qiyou Wang,
  • Tao Luo,
  • Xueying Cao,
  • Yujie Gong,
  • Yuxiang Liu,
  • Yusen Xiao,
  • Hongmei Li,
  • Franz Gröbmeyer,
  • Ying-Rui Lu,
  • Ting-Shan Chan,
  • Chao Ma,
  • Kang Liu,
  • Junwei Fu,
  • Shiguo Zhang,
  • Changxu Liu,
  • Zhang Lin,
  • Liyuan Chai,
  • Emiliano Cortes,
  • Min Liu

摘要

Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO2 reduction reaction (CO2RR) to CO using SAC offers a promising approach for CO2 utilization, but achieving facile CO2 adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO2RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h−1 at 500 mA cm−2. Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO2 conversion efficiency are obtained at 200 mA cm−2 with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO2-to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts.