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<p>Photocatalytic conversion of carbon dioxide (CO<sub>2</sub>) to methanol is hindered by inefficient charge separation and complex multielectron pathways. To address these challenges, we report a synergistic catalyst design in which cobalt vacancies (V<sub>Co</sub>) are coupled with indium single atoms (In SAs). V<sub>Co</sub> sites were precisely constructed on Co<sub>3</sub>O<sub>4</sub> nanosheets using a chlorine cold plasma technique, acting as “atomic sockets” that confine In SAs and form a robust In–O–V<sub>Co</sub> coordination structure. The resulting In/Co<sub>3−<i>x</i></sub>O<sub>4</sub> catalyst delivered a high methanol production rate of 466.7&#xa0;μmol/(g·h) with 92.3% selectivity under simulated solar irradiation, which was eight times greater than that of the vacancy-free catalyst. Mechanistic studies revealed a synergistic functional division: the V<sub>Co</sub> sites efficiently adsorbed and dissociated H<sub>2</sub>O to supply protons, whereas the In SAs polarized CO<sub>2</sub> and stabilized the critical *COOH intermediate. This synergy of strong electronic metal–support interactions improved charge separation and steered the reaction pathway toward methanol, offering a novel atomic-level strategy for designing highly selective CO<sub>2</sub> photoreduction catalysts.</p> Graphical Abstract <p></p>

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Confinement of Indium Single Atoms in Cobalt Vacancies for Enhanced Photocatalytic CO2-to-Methanol Conversion

  • 期刊论文

  • 发表日期：

    2026年4月20日

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  • Yibo Ma,
  • Wan Ni,
  • Jinfeng Zhang,
  • Zhao Wang

摘要

Photocatalytic conversion of carbon dioxide (CO2) to methanol is hindered by inefficient charge separation and complex multielectron pathways. To address these challenges, we report a synergistic catalyst design in which cobalt vacancies (VCo) are coupled with indium single atoms (In SAs). VCo sites were precisely constructed on Co3O4 nanosheets using a chlorine cold plasma technique, acting as “atomic sockets” that confine In SAs and form a robust In–O–VCo coordination structure. The resulting In/Co3−xO4 catalyst delivered a high methanol production rate of 466.7 μmol/(g·h) with 92.3% selectivity under simulated solar irradiation, which was eight times greater than that of the vacancy-free catalyst. Mechanistic studies revealed a synergistic functional division: the VCo sites efficiently adsorbed and dissociated H2O to supply protons, whereas the In SAs polarized CO2 and stabilized the critical *COOH intermediate. This synergy of strong electronic metal–support interactions improved charge separation and steered the reaction pathway toward methanol, offering a novel atomic-level strategy for designing highly selective CO2 photoreduction catalysts.

Graphical Abstract