In-situ restructuring of Ni-based metal organic frameworks for photocatalytic CO<sub>2</sub> hydrogenation.

Gouda, Abdelaziz; Hannouche, Karen; Mohan, Abhinav; Mao, Chengliang; Nikbin, Ehsan; Carrière, Alexandre; Ye, Jessica; Howe, Jane Y et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

As the global quest for sustainable energy keeps rising, exploring novel efficient and practical photocatalysts remains a research and industrial urge. Particularly, metal organic frameworks were proven to contribute to various stages of the carbon cycle, from CO<sub>2</sub> capture to its conversion. Herein, we report the photo-methanation activity of three isostructural, nickel-based metal organic frameworks incorporating additional niobium, iron, and aluminum sites, having demonstrated exceptional CO<sub>2</sub> capture abilities from thin air in previous reports. The niobium version exhibits the highest performance, with a CO<sub>2</sub> to CH<sub>4</sub> conversion rate in the order of 750-7500 µmol*g<sub>catalyst</sub><sup>-1</sup>*h<sup>-1</sup> between 180 °C and 240 °C, achieving 97% selectivity under light irradiation and atmospheric pressure. The in-depth characterization of this framework before and after catalysis reveals the occurrence of an in-situ restructuring process, whereas active surface species are formed under photocatalytic conditions, thus providing comprehensive structure-performance correlations for the development of efficient CO<sub>2</sub> conversion photocatalysts.