Photocatalytic CO2 reduction to C2+ products using a metal–organic framework composited with facet engineered Pd nanoparticles

Abstract

The design of efficient photocatalysts is essential for photocatalytic CO₂ reduction. With the goal of enhancing efficiency to produce C₂₊ products, in this study, we synthesized photocatalysts based on an Fe-MOF composited with facet-engineered palladium nanoparticles (Pd NPs). The synthesis involves in situ reduction of palladium on the surface of the Fe-MOF, namely MIL-100(Fe). When assessing the photocatalytic performance, the synthesized catalyst Pd(111)/MIL-100 exhibits a photoelectron utilization efficiency of 21.4% for converting CO₂ into C₂₊ products, surpassing those in the majority of previously reported studies. The results show that MIL-100(Fe) loaded with Pd NPs that exposed the Pd(111) facet is superior for C₂₊ product selectivity compared with Pd(100)/MIL-100. Density functional theory (DFT) calculations suggest that the difference between Pd(111)/MIL-100 and Pd(100)/MIL-100 may be attributed to the energy barriers required for transition states during the reaction. This study offers an approach for designing photocatalytic catalysts for the CO₂ reduction reaction (CO₂RR) and generating C₂₊ products.