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  4. Photogeneration of Hydrogen: Insights from a Pt(II)-Complex Incorporated into a Covalent Organic Framework
 
research article

Photogeneration of Hydrogen: Insights from a Pt(II)-Complex Incorporated into a Covalent Organic Framework

Gobbato, Thomas
•
Sicignano, Marina
•
Di Vizio, Biagio
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May 13, 2024
Chemcatchem

Pt(II)-based molecular catalysts stand as a prototypical system in hydrogen evolution reactions (HER) owing to their consistently elevated activity levels. Their integration into heterogeneous systems thus provides an ideal platform to develop catalytic materials with optimal atom economy. In this work, by rational molecular design, we have synthesized a novel two-dimensional photoactive Covalent Organic Framework (COF), wherein the pore walls host a quinoline-based alpha-diimine ligand serving as a coordination site for anchoring a Pt(II) molecular catalyst. Thorough structural analyses, employing X-ray photoelectron spectroscopy (XPS), infrared spectroscopy (FT-IR), diffuse reflectance spectroscopy (DR), coupled with DFT calculations, distinctly confirm the Pt(II) complexation through the coordination site of the alpha-diimine ligand. The Pt(II)-metalated COF exhibits photocatalytic activity with a hydrogen evolution rate reaching up to 1300 mu mol g-1 h-1. Nevertheless, the occurrence of platinum nanoparticles in post-catalysis samples, along with reduced photocatalytic activity in the presence of chloride ions, suggests that Pt(II) anchored into the COF backbone might not be the primary catalytic site.|An innovative photoactive covalent organic framework (COF) with pore walls featuring a quinoline-based alpha-diimine ligand as a coordination site was synthesized for anchoring a Pt(II) molecular catalyst for hydrogen evolution reaction (HER). Extensive characterization, supported by DFT calculations, shows that H2 evolution is likely driven by the platinum nanoparticles generated through the photocatalytic processes, rather than by Pt(II) species. image

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Type
research article
DOI
10.1002/cctc.202301732
Web of Science ID

WOS:001219666500001

Author(s)
Gobbato, Thomas
Sicignano, Marina
Di Vizio, Biagio
De Biasi, Federico  
Rosa-Gastaldo, Daniele
Bonetto, Alessandro
Costa, Paolo
Date Issued

2024-05-13

Publisher

Wiley-V C H Verlag Gmbh

Published in
Chemcatchem
Subjects

Physical Sciences

•

Covalent Organic Framework

•

Photocatalysis

•

Hydrogen

•

Molecular Catalysis

•

Platinum Nanoparticles

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LRM  
FunderGrant Number

MIUR- "Dipartimenti di Eccellenza" Grant "NExuS"

University of Padova

European Union - NextGenerationEU

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Available on Infoscience
June 5, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/208322
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