Tuning the selectivity of photothermal CO2 hydrogenation through photo-induced interaction between Ni nanoparticles and TiO2.

Photothermal CO 2 hydrogenation into value-added chemicals driven by abundant solar energy is a promising and sustainable approach for achieving carbon neutralization. Herein, we demonstrate the photo-induced interaction between Ni nanoparticles and TiO 2 support (Ni@TiO 2) for maneuvering the selectivity of photothermal CO 2 hydrogenation. According to experimental characterizations and theoretical simulations, the formed strong metal-support interaction between Ni and TiO 2 can significantly enhance the adsorption of key intermediate *CO for further hydrogenation, thus tuning the CO 2 hydrogenation pathway toward CH 4. Consequently, the Ni@TiO 2 catalyst exhibits a CH 4 production rate of 286.5 mmol g cat −1 h−1 with an 81.8% selectivity under full-spectrum solar light irradiation. Moreover, in situ experimental characterizations and theoretical calculations suggest that photothermal CO 2 hydrogenation over Ni@TiO 2 undergoes a stepwise hydrogenation pathway to methane. This work offers insights into a simple approach for designing efficient nonprecious metal-based CO 2 methanation catalysts. [Display omitted] • A photo-induced approach to construct strong metal-support interaction (SMSI) between Ni and TiO 2 (Ni@TiO 2) is developed. • The selectivity of photothermal CO 2 hydrogenation is rationally maneuvered toward CH 4 production. • The SMSI between Ni and TiO 2 can notably enhance the adsorption of key intermediate *CO for further hydrogenation toward CH 4. • The adsorbed CO and *CHO species are proposed to be the essential intermediates for CO 2 methanation over Ni@TiO 2. [ABSTRACT FROM AUTHOR]