Strong Metal–Support Interaction between Layered Double Oxides and High-Entropy Alloys for the Efficient Light-Driven Dry Reforming of Methane

Dry reforming of methane (DRM) is a promising approach to producing syngas from two greenhouse gases. However, the conventional process requires high temperatures and suffers from low selectivity and stability. Here, we report a highly efficient photothermal DRM catalyst with the feature of strong metal–support interaction (SMSI) in high-entropy alloy (HEA) loaded TiLiAl-based hydrotalcite oxide. Our investigation shows that the reductive TiO2 phase in the support plays a critical role in enabling SMSI, which generates electron transfer from nanoparticles to the support. Such a process creates favorable catalytic sites for molecular activation and promotes photogenerated carrier separation. As a result, this catalyst achieves remarkable H2/CO production rates of 0.55/0.56 mol g–1 h–1 with a balanced selectivity of 0.98 and good stability. This work highlights the importance of regulating metal–support interaction to tailor electron structure and molecular adsorption, providing guidance for the design of highly active photocatalysts toward DRM.