Enhancing Au Active Sites via Heterointerface Reconstruction in Au–Ti Alloy Mesoporous Thin Films for Electrocatalytic Cyclohexene Hydrogenation
Xiaofeng Chen, Linhan Zan, Yueming Shang, Donglin Meng, Xiang Su, Xueliang Xuan, Bin YangABSTRACT
Efficient hydrogenation catalysts are crucial for integrating hydrogen production and storage in organic/water systems. In this study, an AuTiCe/C alloy catalyst with a mesoporous heterostructure was prepared by ion beam sputtering, sequential combined electrochemical dealloying (EDA), and hot pressing, forming a SPE membrane electrode for cyclohexene catalytic hydrogenation. The sequential combined EDA treatment yields low Au loading and high activity. The catalyst exhibits low‐coordinated Au with 0.40 eV lower Au 4f binding energy, ∼1.56% contracted Au(111) spacing, and high‐index Au 2 Ti(103) facets. CeO 2 disperses at grain boundaries of mesoporous walls composed of tetragonal Au 2 Ti and Au. Benefiting from this heterostructure synergy and abundant high‐index facet active sites, cyclohexane conversion reaches 5.96% and hydrogenation current efficiency 50.65% in the organic/water system. DFT calculations confirm the Au 2 Ti/CeO 2 heterostructure yields more thermoneutral ΔGH* and promotes interfacial charge transfer, optimizing adsorption/desorption of intermediates and active H species, synergistically enhancing catalytic hydrogenation. This study provides insights for designing novel Au‐based hydrogenation catalysts and optimizing heterostructure interfaces.