Highly Active Photoreduction of Atmospheric‐Concentration CO2 into CH3COOH over Palladium Particles on Nb2O5 Nanosheets

Abstract The endeavor to drive CO 2 photoreduction towards the synthesis of C 2 products is largely thwarted by the colossal energy hurdle inherent in C−C coupling. Herein, we load active metal particles on metal oxide nanosheets to build the dual metal pair sites for steering C−C coupling to form C 2 products. Taking Pd particles anchored on the Nb 2 O 5 nanosheets as an example, the high‐angle annular dark‐field image and X‐ray photoelectron spectroscopy demonstrate the presence of Pd−Nb metal pair sites on the Pd‐Nb 2 O 5 nanosheets. Density functional theory calculations reveal these sites exhibit a low reaction energy barrier of only 1.02 eV for C−C coupling, implying that the introduction of Pd particles effectively tailors the reaction step to form C 2 products. Therefore, the Pd‐Nb 2 O 5 nanosheets achieve a CH 3 COOH evolution rate of 13.5 μmol g −1 h −1 in photoreduction of atmospheric‐concentration CO 2 , outshining all other single photocatalysts reported to date under analogous conditions.