Graphdiyne Nanospheres as a Wettability and Electron Modifier for Enhanced Hydrogenation Catalysis.

Abstract

Owing to unique alkyne-rich structure, graphdiyne (GDY) has been proven to be a superb support for anchoring metal catalysts. Herein we demonstrate a new role of GDY as the wettability modifier for enhanced hydrogenation catalysis. After loading a certain amount GDY nanospheres, the silica mesoporous channels become superaerophilic, which allows gaseous H2 to be directly stored inside, thus significantly increasing the H2 concentration around the palladium nanoparticles (NPs). At the same time, GDY nanospheres also alter the electronic structure of the Pd NPs via a strong d-π interaction. Combining these two roles of GDY, allows the hydrogenation of benzaldehyde to proceed under ambient H2 pressure in water, with an impressive 4.3-fold enhancement compared to the unmodified Pd/mSiO2 catalyst. This study demonstrates a new role of GDY in constructing wettability matched catalysts for gas-liquid-solid tri-phase reactions.