Unlocking Methane Generation via Photo‐Thermal‐Coupled CO ₂ Hydrogenation by Integrating FeNiCrMnCo Multicomponent Alloy with GaN Nanowires

Abstract The exploration of a noble‐metal‐free photo‐thermal‐coupled catalytic architecture plays a vital role in solar‐driven conversion of carbon dioxide (CO ₂ ) into high‐value fuels and chemicals. In this study, FeNiCrMnCo multicomponent alloy (MCA) is integrated with GaN nanowires (NW's) for photo‐thermal‐coupled catalytic CO ₂ methanation. The MCA/GaN NW's nanohybrid demonstrates a considerable methane production rate of 199 mmol∙g ⁻¹ ∙h ⁻¹ with an impressive selectivity of 93% under white light irradiation of 3 W∙cm ⁻² at 290 °C by external heating. The turnover number approaches 20,160 mole CH ₄ per mole of MCA over a continuous operation period of 120 h, showcasing remarkable stability. Mechanistic investigations reveal that the unique MCA provides a flexible platform for tailoring the electronic and catalytic properties to optimize the adsorption and activation of CO₂ and H₂, thus leading to efficient and selective CO₂ methanation. This study presents an industry‐friendly architecture for photo‐thermal‐coupled CO ₂ hydrogenation into high‐value fuels and chemicals by coupling a noble‐metal‐free multicomponent alloy with GaN NWs, paving the way for advancements in sustainable energy conversion through CO ₂ utilization.