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 H 2 to be directly stored inside, thus significantly increasing the H 2 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 H 2 pressure in water, with an impressive 4.3‐fold enhancement compared to the unmodified Pd/mSiO 2 catalyst. This study demonstrates a new role of GDY in constructing wettability matched catalysts for gas‐liquid‐solid tri‐phase reactions.