4.8 Article

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

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 34, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202207255

Keywords

Graphdiyne; Heterogeneous Catalysis; Hydrogenation; Palladium nanoparticles; Wettability

Funding

  1. National Key R&D Program of China [2018YFA0703503]
  2. National Natural Science Foundation of China [NSFC 21932006, 92161112]
  3. Beijing National Laboratory for Molecular Sciences [BNLMS-CXXM-202103]
  4. Youth Innovation Promotion Association of CAS [Y2017049]

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GDY can serve as a wettability modifier to enhance hydrogenation catalysis, and the modified catalyst shows improved performance in gas-liquid-solid tri-phase reactions.
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-pi 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.

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