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

Abstract Interface engineer of Ru‐based catalysts has become an attractive strategy to improve ammonia (NH ₃ ) 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 NH ₃ 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 NH ₃ and induces the generation of medium‐strong basic sites, which contributed to N ₂ 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 NH ₃ decomposition, offering a valuable reference for the construction of highly active interface on Ru‐based catalysts.