Directly Integrating Ni–NiO Nanoparticles Into Silicalite‐1 to Boost Photothermal CO ₂ Methanation

ABSTRACT Photothermal carbon dioxide (CO 2 ) hydrogenation offers an effective avenue to produce solar fuel like methane (CH 4 ) by using the entire sunlight spectrum. However, its application is severely hindered by the sluggish kinetics, leading to the low solar‐to‐chemical (STC) energy conversion efficiency. Herein, we demonstrated a strategy to boost the photothermal CO 2 conversion by directly integrating a high loading (>10 wt.%) of Ni–NiO species into silicalite‐1. The highly dispersive Ni species effectively harvested the full solar spectrum to reach a remarkable photothermal effect. Simultaneously, the NiO and Ni sites facilitate CO 2 and H 2 activation, respectively, reducing the energy barrier. The surrounding silicalite‐1 matrix functions as a thermally insulation shell and exerts a confinement effect to enrich the key intermediate CO. Thereby, under atmospheric conditions, an unprecedented CO 2 conversion rate of 92.7 mol m −2 h −1 (2.7 mol g cat −1 h −1 and 23.0 mol g Ni −1 h −1 ) was obtained to achieve a remarkable STC of 9.1%.