Efficient photothermal CO₂ methanation over Ni nanoparticles on oxygen-deficient V₂O₃ via strong metal-support interaction

Photothermal catalysis offers a sustainable route for CO2 utilization by directly converting solar energy into chemical fuels. Herein, we demonstrate the rational design of an oxygen vacancy-rich Ni/V2O3 catalyst featuring strong metal-support interaction (SMSI) for efficient photothermal CO2 methanation. The catalyst achieves a CO2 conversion of 84.3% with nearly 100% CH4 selectivity under 2.43 W cm−2 irradiation, and maintains structural and catalytic stability over 50 h of continuous operation. Multimodal characterizations reveal that the V2O3 support provides broad-spectrum light absorption and efficient photothermal conversion, while its abundant oxygen vacancies promote CO2 adsorption and activation. Simultaneously, SMSI at the Ni-V2O3 interface modulates the local electronic structure and facilitates H2 dissociation and spillover. In situ diffuse reflectance infrared Fourier transform spectroscopy and temperature-programmed studies confirm the formation of key intermediates and highlight the synergistic interplay between vacancies and SMSI in promoting CO2 hydrogenation. This work demonstrates an effective interfacial engineering strategy for developing high-performance photothermal catalysts for solar-driven CO2 conversion.