Optimization of Fe/Ni organic frameworks with core–shell structures for efficient visible-light-driven reduction of carbon dioxide to carbon monoxide

To address CO₂ emissions caused by the overuse of fossil fuels, photocatalytic CO₂ reduction from metal-organic frameworks (MOFs) to valuable chemicals is critical for energy conversion and storage. Core-shell MOFs improve interfacial interactions, increasing the number of active sites in the catalyst, thereby improving the photocatalytic reduction. In this work, the catalytic performance of Fe/Ni-MOFs toward photocatalytic CO₂ reduction was improved using a bimetallic strategy. We successfully synthesized a series of Fe/Ni-MOFs with a core-shell structure using a single-step approach combined with hydrothermal synthesis. By altering the synthesis conditions of the bimetallic organic skeleton and contrasting it with a single MOF, we successfully synthesized Fe/Ni-T120 through an efficient photocatalytic reduction of CO₂. The results of photocatalytic CO₂ reduction experiments indicated that upon using [Ru(bpy)₃]Cl₂·6H₂O as a photosensitizer and triethanolamine (TEOA) and acetonitrile (MeCN) as sacrificial agents, the CO evolution rate of Fe/Ni-T120 reached 9.74 mmol g^-1 h^-1 and the CO₂ to CO selectivity reached up to 92.1%. Additionally, Fe/Ni-T120 has a broad response range to visible light, a high photocurrent intensity, good chemical stability, and strong photocatalytic efficiency, even after repeated cycles. This study proposes a straightforward method for producing adaptable and stable MOFs for effective photocatalytic CO₂ reduction that is driven by visible light.