Laser‐driven Plasma Synthesis of CeO ₂ ‐bridged Ni Nanoparticles for Efficient and Stable Photothermal CO ₂ Methanation

ABSTRACT Photothermal catalytic CO 2 methanation provides a promising route toward realizing carbon recycling. However, conventional supported Ni‐based photothermal catalysts are limited by inadequate CO 2 activation capability and severe sintering of Ni nanoparticles at high temperatures. Here, a bead‐like CeO 2 ‐bridged Ni nanoparticle catalyst (Ni‐CeO 2 ‐Ni) is constructed via a laser‐driven plasma synthesis strategy, in which Ni nanoparticles are bridged by CeO 2 layers to form a cohesive bonded interface. The catalyst delivers exceptional performance in photothermal CO 2 methanation, achieving a CH 4 STY of 1.32 mol·g cat −1 ·h −1 and up to 99% selectivity at 350°C with a WHSV of 200 000 mL·g cat −1 ·h −1 , while maintaining stability for 140 h. Mechanistic studies reveal that the unique bridged interface between CeO 2 and Ni enhances CO 2 adsorption and activation by modulating electron transfer to upshift the Ni d‐band center. In addition, this structure provides abundant interfacial sites with enhanced sintering resistance, boosting overall catalytic efficiency and stability. More importantly, the Ni‐CeO 2 ‐Ni catalyst enables solar‐driven photothermal CO 2 methanation under natural sunlight, achieving a CH 4 production rate of 1.15 mol·g cat −1 ·h −1 at a solar irradiance of 0.49 kW·m −2 during winter. This work demonstrates that rational interfacial engineering can yield photothermal CO 2 methanation catalysts with both high activity and robust stability.