Potassium‐Modulated Ni/Carbon Catalyst for Efficient Photothermal CO ₂ Reduction: Unveiling the Role of Electronic Metal–Support Interactions

Abstract With the intensification of the greenhouse effect, the catalytic conversion of CO 2 has emerged as a critical challenge. Photothermal catalytic CO 2 conversion into value‐added products offers a promising strategy to mitigate CO 2 emissions. In this study, a carbon‐based catalyst loaded with metallic nickel is developed for efficient photothermal reduction of CO 2 to CO. Potassium (K) modification is further introduced by tuning the K doping content, and the optimized catalyst exhibits exceptional CO selectivity (≈100%) and photothermal activity (266 mmol g −1 h −1 ). Mechanistic investigations reveal that K modification significantly enhances CO 2 adsorption capacity and modulates electron transfer pathways, as supported by DFT calculations. The synergistic effect of K modification in promoting CO 2 activation and electron‐carrier interactions under photothermal conditions is demonstrated to be pivotal for driving the CO 2 to CO conversion. This work clarifies the role of alkali metal modification in photo‐thermal catalytic systems and establishes a structure‐performance relationship guided by electron‐interface engineering.