Elucidating the Role of Ru‐O _v ‐Ce Interfacial Structure on Ru/Silicate‐1 Catalyst by the Doping of CeO ₂ for Ammonia Decomposition

Interface engineer of Ru-based catalysts has become an attractive strategy to improve ammonia (NH₃) decomposition performance by precisely modulating the microenvironment of Ru site. Therefore, the Ru-O_v-Ce interfacial structure is constructed on Silicate-1 (S-1) to improve the NH₃ decomposition performance of Ru/S-1 catalyst. The activity test suggests that the generation of Ru-O_v-Ce interfacial structure considerably improved the catalytic performance of Ru/S-1 catalyst, boosting the specific activity from 2546.7 to 4461.3 h^-1 at 450 °C, and displays promising cycle and long-term stability. Comprehensive characterization results reveal that Ru-O_v-Ce interfacial structure is favorable for enhancing metal-support interaction, inducing the generation of oxygen vacancies, and optimizing the electronic structure of Ru species. Moreover, Ru-O_v-Ce interfacial structure exhibits favorable adsorption performance for NH₃ and induces the generation of medium-strong basic sites, which contributed to N₂ desorption. Furthermore, the in situ DRIFTS and DFT calculations reveal that Ru-O_v-Ce interfacial structure performed superbly in the cleavage of N-H bonds and N* and H* recombination, which greatly lowers the reaction energy barriers and improves the reaction kinetics. This work thoroughly explores the specific action mechanisms of superior Ru-O_v-Ce interfacial structure in NH₃ decomposition, offering a valuable reference for the construction of highly active interface on Ru-based catalysts.