pH‐Mediated Strong Metal‐Support Interaction Construction Through Dynamic Fermi Level Tuning

ABSTRACT The metal–support interface is central to governing catalytic transformations. While strong metal–support interaction (SMSI) is an established strategy to tailor the morphology and electronic properties of supported metal catalysts, the role of interfacial charge redistribution in SMSI formation remains poorly understood and rarely leveraged. Here, we report a dual‐stimuli approach that combines pH modulation with ultrasonication to mediate SMSI construction in aqueous solution through dynamic Fermi level tuning. By leveraging in situ pH‐driven charge redistribution at the metal–support interface, we achieve controllable SMSI encapsulation of metal nanoparticles, as verified by electrochemical analysis, work function measurements, and x‐ray‐based techniques. The resulting catalysts exhibit tunable SMSI features and deliver enhanced activity and selectivity in hydrogenation reactions. This work establishes a facile strategy to modulate catalyst structure and electronic properties by exploiting Fermi level variation as a driving force, thereby advancing rational SMSI design and catalytic performance across diverse environments.