posted on 2020-11-13, 15:40authored byChidharth Krishnaraj, Himanshu Sekhar Jena, Laurens Bourda, Andreas Laemont, Pradip Pachfule, Jérôme Roeser, C. Vinod Chandran, Sander Borgmans, Sven M. J. Rogge, Karen Leus, Christian V. Stevens, Johan A. Martens, Veronique Van Speybroeck, Eric Breynaert, Arne Thomas, Pascal Van Der Voort
Photocatalytic
reduction of molecular oxygen is a promising route
toward sustainable production of hydrogen peroxide (H2O2). This challenging process requires photoactive semiconductors
enabling solar energy driven generation and separation of electrons
and holes with high charge transfer kinetics. Covalent organic frameworks
(COFs) are an emerging class of photoactive semiconductors, tunable
at a molecular level for high charge carrier generation and transfer.
Herein, we report two newly designed two-dimensional COFs based on
a (diarylamino)benzene linker that form a Kagome (kgm) lattice and show strong visible light absorption. Their high crystallinity
and large surface areas (up to 1165 m2·g–1) allow efficient charge transfer and diffusion. The diarylamine
(donor) unit promotes strong reduction properties, enabling these
COFs to efficiently reduce oxygen to form H2O2. Overall, the use of a metal-free, recyclable photocatalytic system
allows efficient photocatalytic solar transformations.