Interfacial\nRegulation of Ru-Based Catalysts for the\nEnhanced Activity of Ammonia Decomposition

Ru-based catalysts feature an intrinsic activity toward\nNH<sub>3</sub> decomposition, while their catalytic mechanism associated\nwith the interface with support remains elusive. Herein, with the\ninterfacial regulation of Ru catalysts by TiO<sub>2</sub> via strong\nmetal–support interactions (SMSI), i.e., Ru/TiO<sub>2</sub>, an enhanced activity of NH<sub>3</sub> decomposition can be realized\nwith a turnover frequency of hydrogen production 2-fold higher than\nthat on Ru/SiO<sub>2</sub>. With characterizations and density functional\ntheory calculations, the newly generated Ru/TiO<sub>2–<i>x</i></sub> interface with the electron-rich Ru sites was proven\nto not only facilitate the adsorption of ammonia and its N–H\nbond cleavage but also promote the associative desorption of N* species.\nMoreover, the poisoning kinetics of hydrogen during reactions can\nalso be alleviated due to the associative desorption of H* occurring\nprimarily on the residual Ru surface. This work demonstrates that\ninterfacial regulation provides an efficient strategy for the catalytic\nactivity modulation of Ru-based catalysts especially in NH<sub>3</sub> decomposition.