Reactant enrichment in hollow void of Pt NPs@MnOx nanoreactors for boosting hydrogenation performance.

Abstract

In confined mesoscopic spaces, the unraveling of a catalytic mechanism with complex mass transfer and adsorption processes such as reactant enrichment is a great challenge. In this study, a hollow nanoarchitecture of MnOx-encapsulated Pt nanoparticles was designed as a nanoreactor to investigate the reactant enrichment in a mesoscopic hollow void. By employing advanced characterization techniques, we found that the reactant-enrichment behavior is derived from directional diffusion of the reactant driven through the local concentration gradient and this increased the amount of reactant. Combining experimental results with density functional theory calculations, the superior cinnamyl alcohol (COL) selectivity originates from the selective adsorption of cinnamaldehyde (CAL) and the rapid formation and desorption of COL in the MnOx shell. The superb performance of 95% CAL conversion and 95% COL selectivity is obtained at only 0.5MPa H2 and 40min. Our findings showcase that a rationally designed nanoreactor could boost catalytic performance in chemoselective hydrogenation, which can be of great aid and potential in various application scenarios.