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.