4.6 Article

Local charge transfer within a covalent organic framework and Pt nanoparticles promoting interfacial catalysis

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 12, Issue 10, Pages 3240-3246

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cy02024b

Keywords

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Funding

  1. National Key Research and Development Program of China [2020YFA0710303]
  2. National Natural Science Foundation of China [52172188, U1905215, 52072076]
  3. Natural Science Foundation of Fujian Province of China [2019J01226]

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By synthesizing a pyridine-functionalized covalent organic framework (COF), the stability and electronic density of platinum nanoparticles (Pt NPs) were enhanced, leading to improved catalytic activity in the hydrolysis of ammonia borane (AB) for hydrogen production. This study advances the application of covalent organic frameworks in heterogeneous catalysis.
Striking a balance between the stability and activity of metal nanoparticles (NPs) is crucial in designing efficient heterogeneous catalysts. This challenge requires supporters with highly tunable behaviour enabling metal active sites with appropriate electronic properties. Herein, we demonstrate a newly synthesized pyridine-functionalized covalent organic framework (COF) rendering Pt NPs with enhanced stability and electronic density. Periodic channels with pendant pyridine groups can efficiently stabilize Pt NPs as active sites. Local charge transfer from the COF to Pt was confirmed by experimental and theoretical methods. The increased electron density on Pt promotes the rate-limiting cleavage of the O-H band in H2O, resulting in enhanced catalytic activity for the hydrolysis of ammonia borane (AB) for H-2 production compared to other non-pyridine-functionalized COF-based catalysts. The mechanistic insights into the local charge transfer advance the applicability of COFs for heterogeneous catalysis.

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