Wei Guo, Guoqiang Zhao, Mingxia Gao, Hongge Pan, Wenping Sun
Abstract Strong metal‐support interaction (SMSI) critically regulates the catalytic performance of supported metal catalysts. Conventionally, a high‐temperature reduction (HTR) in H 2 is required to construct this state, a process that involves H 2 dissociation, spillover, and support activation. However, while a high temperature is indispensable to initiate SMSI, it also risks sintering the metal species, presenting a fundamental dilemma. Here, we demonstrate that this challenge can be overcome by accelerating the hydrogen catalysis kinetics through strategically manipulating active metal sites. As a proof of concept, by introducing Pt single atoms, the HTR temperature required to construct SMSI between Ru nanoparticles and TiO 2 is reduced from 600 to 400 °C. The key is that the Pt sites substantially promote the hydrogen spillover from Ru to TiO 2 , which is inherently sluggish due to an over‐strong Ru–H interaction. Both experimental and theoretical results confirm the accelerated support activation with the presence of Pt. The general effectiveness of this strategy is further validated by promoting SMSI formation in a Pd/TiO 2 system. The results highlight the significant role catalysis plays in SMSI manipulation and provide deeper insights into the SMSI formation mechanism, which is vital to the advancement of supported metal catalysts and beyond.