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<p>The CO<sub>2</sub> photoreduction into CH<sub>4</sub> not only promotes the carbon cycle but also generates important chemical raw materials. Although the CH<sub>4</sub> formation has a thermodynamic advantage compared to CO, its selectivity depends on the kinetically stable adsorption of *CO intermediates and the sufficient supply of *H intermediates. We initially summarize the significant advances in detecting the dynamic evolution of active sites and capturing the transient intermediates via <i>in situ</i> characterization and theoretical calculations, analyzing the characteristics of catalysts with high CH<sub>4</sub> selectivity and providing guidance for CH<sub>4</sub> formation. Moreover, we review strategies of optimizing the reduction sites to promote the CO<sub>2</sub> adsorption, regulate the intermediate evolution, and enable the regeneration of reduction sites, ensuring the stable adsorption of *CO intermediates and enhancing CH<sub>4</sub> selectivity. Furthermore, we review the optimization of oxidation sites to accelerate *H generation, *H migration, and regeneration of oxidation sites, ensuring an adequate *H supply and improving the CH<sub>4</sub> selectivity. Finally, by analyzing the limitations of current research, we provide guiding suggestions for improving the selectivity of CO<sub>2</sub> photoreduction into CH<sub>4</sub>.</p>

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Design of surface redox reactions for improving the selectivity of CO2 photoreduction into CH4

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Chenjin Huang,
  • Yongfu Sun,
  • Yi Xie

摘要

The CO2 photoreduction into CH4 not only promotes the carbon cycle but also generates important chemical raw materials. Although the CH4 formation has a thermodynamic advantage compared to CO, its selectivity depends on the kinetically stable adsorption of *CO intermediates and the sufficient supply of *H intermediates. We initially summarize the significant advances in detecting the dynamic evolution of active sites and capturing the transient intermediates via in situ characterization and theoretical calculations, analyzing the characteristics of catalysts with high CH4 selectivity and providing guidance for CH4 formation. Moreover, we review strategies of optimizing the reduction sites to promote the CO2 adsorption, regulate the intermediate evolution, and enable the regeneration of reduction sites, ensuring the stable adsorption of *CO intermediates and enhancing CH4 selectivity. Furthermore, we review the optimization of oxidation sites to accelerate *H generation, *H migration, and regeneration of oxidation sites, ensuring an adequate *H supply and improving the CH4 selectivity. Finally, by analyzing the limitations of current research, we provide guiding suggestions for improving the selectivity of CO2 photoreduction into CH4.