Red edge effect and chromoselective photocatalysis with amorphous covalent triazine-based frameworks

Yajun Zou, Sara Abednatanzi, Parviz Gohari Derakhshandeh, Stefano Mazzanti, Christoph M. Schüßlbauer, Daniel Cruz, Pascal Voort, Jian-Wen Shi, Markus Antonietti, Dirk M. Guldi and Aleksandr Savateev ()
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Yajun Zou: Max Planck Institute of Colloids and Interfaces
Sara Abednatanzi: Ghent University
Parviz Gohari Derakhshandeh: Ghent University
Stefano Mazzanti: Max Planck Institute of Colloids and Interfaces
Christoph M. Schüßlbauer: Friedrich-Alexander University Erlangen-Nürnberg
Daniel Cruz: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Pascal Voort: Ghent University
Jian-Wen Shi: Xi’an Jiaotong University
Markus Antonietti: Max Planck Institute of Colloids and Interfaces
Dirk M. Guldi: Friedrich-Alexander University Erlangen-Nürnberg
Aleksandr Savateev: Max Planck Institute of Colloids and Interfaces

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: Abstract Chromoselective photocatalysis offers an intriguing opportunity to enable a specific reaction pathway out of a potentially possible multiplicity for a given substrate by using a sensitizer that converts the energy of incident photon into the redox potential of the corresponding magnitude. Several sensitizers possessing different discrete redox potentials (high/low) upon excitation with photons of specific wavelength (short/long) have been reported. Herein, we report design of molecular structures of two-dimensional amorphous covalent triazine-based frameworks (CTFs) possessing intraband states close to the valence band with strong red edge effect (REE). REE enables generation of a continuum of excited sites characterized by their own redox potentials, with the magnitude proportional to the wavelength of incident photons. Separation of charge carriers in such materials depends strongly on the wavelength of incident light and is the primary parameter that defines efficacy of the materials in photocatalytic bromination of electron rich aromatic compounds. In dual Ni-photocatalysis, excitation of electrons from the intraband states to the conduction band of the CTF with 625 nm photons enables selective formation of C‒N cross-coupling products from arylhalides and pyrrolidine, while an undesirable dehalogenation process is completely suppressed.

Date: 2022
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DOI: 10.1038/s41467-022-29781-9

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