Engineering uranyl sites into MOFs for efficient and highly selective photocatalytic CO2 reduction

Abstract

Utilizing sunlight for the photocatalytic reduction of CO₂ to CO and other high value-added products represents a pivotal strategy for environment protection and mitigation of the energy crisis. Herein, we have designed and prepared a uranium-based organic-framework (MOF), IHEP-101, featuring a uranyl photocatalytic active center, engineered for the efficient photocatalytic reduction of CO₂. Demonstrating exceptional activity, IHEP-101 achieves a CO production rate of up to 458 μmol g⁻¹ h⁻¹. The mechanism underlying IHEP-101's photocatalytic CO₂ reduction is thoroughly detailed through in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) and theoretical calculations. This study underscores the effectiveness of UO₂²⁺ cations as active sites for the photocatalytic reduction of CO₂, introducing an innovative method for designing and synthesizing highly efficient photocatalysts aimed at CO₂ reduction.