Bioinspired Hollow Nanoreactor: Catalysts that Carry Gaseous Hydrogen for Enhanced Gas-Liquid-Solid Three-Phase Hydrogenation Reactions

摘要

For conventional gas-liquid-solid three-phase heterogeneous hydrogenation reactions, hydrogen must be dissolved into the solvent to be a participating reactant, restricting the reaction rates. In this study, we demonstrate that gaseous hydrogen could be directly involved in gas-liquid-solid hydrogenation reactions through a bioinspired hollow nanoreactor with superaerophilic surface to enhance the reaction rates. We produce Pd@meso-SiO2 hollow nanoreactor, whose external surface is modified with perfluorodecyltriethoxysilane (PFDTS). In aqueous solutions, H-2 gas could be spread quickly on the surface and stored in the cavity of hollow spheres, and participated in hydrogenation reactions, thereby enhancing H-2 concentration around Pd nanoparticles. In hydrogenation of olefin reactions, such three-phase interface allows rapid and direct transportation of H-2 bubbles to the surface of Pd nanoparticles rather than through diffusion of dissolved H-2 in liquid phase, leading to an enhanced catalytic rate. This strategy is expected to be useful for designing and developing new catalytic systems of gas-liquid-solid three-phase reaction.