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

Abstract

Ru-based catalysts feature an intrinsic activity toward NH 3 decomposition, while their catalytic mechanism associated with the interface with support remains elusive. Herein, with the interfacial regulation of Ru catalysts by TiO 2 via strong metal–support interactions (SMSI), i.e., Ru/TiO 2, an enhanced activity of NH 3 decomposition can be realized with a turnover frequency of hydrogen production 2-fold higher than that on Ru/SiO 2 . With characterizations and density functional theory calculations, the newly generated Ru/TiO 2– 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 NH 3 decomposition.