Interfacial structure engineering enhances photo-thermal CO2 hydrogenation over Ni-CeO2 nanocomposites

Abstract

Metal-support interfaces play pivotal roles in governing the catalytic behaviors in heterogeneous catalysts, yet their optimized construction remains a formidable challenge. Here, we delve into the role of nickel-ceria interfaces in enhancing photo-thermal CO₂ hydrogenation by designing a series of Ni/CeO₂ composite catalysts with distinct interfacial features. The one with a well-defined nickel-ceria interface, achieved through lattice matching, demonstrates an exceptional CH₄ production rate of 477.3 mmol g_cat⁻¹ h⁻¹ (99.7% selectivity, 89.4% CO₂ conversion) at 250°C under ambient pressure and light irradiation (200–1,100 nm, 2740 mW cm⁻²). This remarkable performance is credited to the distinctive metal-support interaction and efficient charge transfer at the interface. In contrast, catalysts lacking lattice-matched interfaces or featuring encapsulated nickel nanoparticles show inferior activity due to inhibited charge transfer and restricted access to active sites. These findings underscore the importance of interface engineering in optimizing photo-thermal catalysts for CO₂ hydrogenation.