Synergistic Pd sites in ordered macroporous In2O3 for enhanced CO2 photo-reduction

Solar-driven conversion of carbon dioxide (CO₂) and water (H₂O) into carbon-based fuels and high-value-added chemicals represents a promising sustainable strategy for achieving recycling of carbon resources. Achieving efficient photocatalytic CO₂ reduction using H₂O as a hydrogen source requires the synergisticoptimization of both charge and proton transfer between CO₂ reduction and H₂O oxidationhalf-reactions.The integration of complementary metal single‐atom andclusters on photocatalystscan establish multiple catalyticcenters, potentially synergizing to improve both the half-reactions.

Recently, a research team led by Prof. Benxia Li (Zhejiang Sci-Tech University) designed a Pd_1+c/3DOM-In₂O₃ catalyst by engineering synergistic Pd₁ and Pd_c sites in 3DOM-In₂O₃ framework. The innovative integration of synergistic Pd₁‐Pd_c sites with unique LSPR property and the 3DOM structures enableshighly efficient conversion of CO₂ and H₂O into CO.The results were published in Chinese Journal of Catalysis (DOI: 10.1016/S1872‐2067(25)64919‐9).

The Pd_1+c/3DOM-In₂O₃ catalyst was synthesized through template‐assisted in‐situ pyrolysis followed by thermal treatment in a mixed H₂/Ar atmosphere. The co-existence of Pd single atoms and clusters not only offers synergistic active sites to simultaneously promote the reaction of CO₂ and H₂O, but also significantly improves the separation and transfer efficiencies of photogenerated electrons and holes. Under simulated sunlight irradiation, the surface temperature of the catalyst rapidly rises to approximately 230 °C due to the photothermal effect of Pd clusters. This generated thermal energy further enhances the photocatalytic conversion of CO₂ and H₂O, achieving a CO production rate of 192.52 μmol g^–1 h^–1 with a selectivity of 88.51%.

Density functional theory (DFT) calculations reveal that Pd clusters substantially reduce the thermodynamic energy barrier of H₂O dissociation, thereby accelerating proton‐coupled electron transfer for CO₂ reduction. Pd single atoms serve as the optimal active sites for the selective conversion of CO₂ into CO, while the presence of Pd clusters enhances the adsorption and activation of CO₂ at these Pd single‐atom sites. The synergistic interaction between Pd single atoms and clusters, along with the integration of photocatalysis and photothermal effect, significantly improves the CO₂ and H₂O conversion to CO.

About the journal

Chinese Journal of Catalysis is co-sponsored by Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Chinese Chemical Society, and it is currently published by Elsevier group. This monthly journal publishes in English timely contributions of original and rigorously reviewed manuscripts covering all areas of catalysis. The journal publishes Reviews, Accounts, Communications, Articles, Highlights, Perspectives, and Viewpoints of highly scientific values that help understanding and defining of new concepts in both fundamental issues and practical applications of catalysis. Chinese Journal of Catalysis ranks among the top six journals in Applied Chemistry with a current SCI impact factor of 17.7.

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