Tuning the H₂ Adsorption Capacity of Au/TiO₂ Catalysts to Enable

New Hydrogenation and Hydrogenolysis Chemistries

Bert D. Chandler,

Pennsylvania State University

            Supported Au nanoparticle (NP) catalysts, which are composed of small (< 5 nm) Au NPs on a (typically) metal oxide carrier, have desirable selectivity for several industrially important reactions; however, they suffer from extremely low activity associated with weak H₂ adsorption onto the catalyst.  Several recent discoveries indicate H₂ adsorbs on Au catalysts at the metal-support interface (MSI), reversibly transferring the protons and electrons to the support.  The thermodynamics and kinetics of this process are not well understood and offer new opportunities for catalyst design if they can be properly characterized and controlled.  This project will improve our fundamental understanding of these processes by (i) characterizing the roles of surface basicity, Au electronics, and support reducibility in influencing this chemistry; (ii) develop and test near-surface support compositions that will allow us to control and tune both the H₂ adsorption capacity and adsorption strength of the support; and (iii) add secondary surface reaction centers that can utilize the transferred H-atom equivalents to improve several industrially important catalytic reactions and develop new approaches to several catalytic chemistries.  Collectively, these studies will develop catalysts capable of activating H₂ at the MSI, transport it across the support as protons and electrons, and transfer the reducing equivalents to hydrogenation targets.