Pyrene and Bipyridine-based Covalent Triazine Framework as Versatile Platform for Photocatalytic Solar Fuels Production

ChemRxiv

Abstract

The ability to molecularly engineer materials may be one of the most powerful tools in favor of high performing heterogeneous catalysts. Porous organic polymers stand out as photocatalysts due to their high chemical stability, outstanding optoelectronic properties and their easy and tunable syntheses. In photocatalysis, the insertion of photosensitizing π-extended molecules into a molecularly well-defined donor-acceptor junctions is supposed to increase the cata-lytic activity, but yet remain experimentally underdeveloped. Here, we present a pyrene-based Covalent Triazine Framework (CTF) synthesized through a polycondensation approach, which was designed to contain a molecularly defined pyrene-triazine-bipyridine donor-acceptor-acceptor triad as the repetition unit of the CTF. The CTF is an efficient photocatalyst for hydrogen evolution from water reaching a production rate of 61.5 mmolH2/h/gcat. Moreover, the same CTF can easily be used as porous macroligand for an organometallic Rh complex to efficiently catalyze the carbon dioxide photoreduction into formic acid under visible light.

Authors 11

1. Marcelo A. Fávaro Aachen Institut für Technische und Makromolekulare Chemie

   Lyon 1 Université · Centre National de la Recherche Scientifique · Université de Lyon · Institut de Recherches sur la Catalyse et l'Environnement de Lyon · RWTH Aachen University

   Affiliation as printed

   Institut für Technische und Makromolekulare Chemie, RWTH Aachen University

   Université de Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON - UMR 5256

2. Jin Yang

   Technische Universität Berlin

   Affiliation as printed

   Fakultät II Institut für Chemie, Technische Universität Berlin

3. Daniel Ditz Aachen Institut für Technische und Makromolekulare Chemie

   RWTH Aachen University

   Affiliation as printed

   Institut für Technische und Makromolekulare Chemie, RWTH Aachen University

4. Hüseyin Küçükkeçeci

   Technische Universität Berlin

   Affiliation as printed

   Fakultät II Institut für Chemie, Technische Universität Berlin

5. Mohammed H. Alkhurisi

   University of Regensburg

   Affiliation as printed

   Institute of Inorganic Chemistry, University of Regensburg

6. Sebastian Bergwinkl

   University of Regensburg

   Affiliation as printed

   Institute of Physical and Theoretical Chemistry, University of Regensburg

7. Arne Thomas

   Technische Universität Berlin

   Affiliation as printed

   Fakultät II Institut für Chemie, Technische Universität Berlin

8. Elsje Alessandra Quadrelli

   Lyon 1 Université · Centre National de la Recherche Scientifique · Université de Lyon · Institut de Recherches sur la Catalyse et l'Environnement de Lyon

   Affiliation as printed

   Université de Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON - UMR 5256

9. Regina Palkovits Aachen Institut für Technische und Makromolekulare Chemie

   Max Planck Institute for Chemical Energy Conversion · RWTH Aachen University

   Affiliation as printed

   Institut für Technische und Makromolekulare Chemie, RWTH Aachen University

   Max-Planck-Institute for Chemical Energy Conversion

10. J. Canivet

    Lyon 1 Université · Centre National de la Recherche Scientifique · Université de Lyon · Institut de Recherches sur la Catalyse et l'Environnement de Lyon

    Affiliation as printed

    Université de Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON - UMR 5256

11. Florian M. Wisser

    University of Regensburg

    Affiliation as printed

    Institute of Inorganic Chemistry, University of Regensburg