Manipulating the Microenvironment of Surfactant-Encapsulated Pt Nanoparticles to Promote Activity and Selectivity
Gengnan Li, Nebojša Marinković, Bin Wang, Mallikharjuna Rao Komarneni, Daniel E. Resasco
Abstract
Precise tuning of the local environment surrounding the active site is key to engineering catalytic materials. Here, we have explored a nanoconfined catalytic system that exhibits highly selective hydrogenation of C=O bonds relative to C=C bonds. Organic surfactants anchored on metal surfaces not only can modify the catalytic performance according to their steric properties but can also regulate the solvent distribution at the liquid–solid interface, creating nanopockets of adjustable hydrophobic/hydrophilic interactions. The cooperative action of organic ligands and water molecules leads to catalytic pathways distinct from those on catalysts without functionalization. By combining precise catalyst synthesis with in situ spectroscopic characterization, reaction kinetics analysis, and computational techniques, this study provides a quantitative description of a catalyst with a tunable local environment near the active site. This precise control is reminiscent of that of natural enzymes that can alter their scaffold structure to adjust the solvent composition in their inner cavities and control reaction selectivity.