Interfacial Regulation of Ru-Based Catalysts for the Enhanced Activity of Ammonia Decomposition

Ru-based catalysts feature an intrinsic activity toward NH3 decomposition, while their catalytic mechanism associated with the interface with support remains elusive. Herein, with the interfacial regulation of Ru catalysts by TiO2 via strong metal–support interactions (SMSI), i.e., Ru/TiO2, an enhanced activity of NH3 decomposition can be realized with a turnover frequency of hydrogen production 2-fold higher than that on Ru/SiO2. With characterizations and density functional theory calculations, the newly generated Ru/TiO2–x interface with the electron-rich Ru sites was proven to not only facilitate the adsorption of ammonia and its N–H bond cleavage but also promote the associative desorption of N* species. Moreover, the poisoning kinetics of hydrogen during reactions can also be alleviated due to the associative desorption of H* occurring primarily on the residual Ru surface. This work demonstrates that interfacial regulation provides an efficient strategy for the catalytic activity modulation of Ru-based catalysts especially in NH3 decomposition.