Integrating Bifunctionality and Chemical Stability in Covalent Organic Frameworks via One-Pot Multicomponent Reactions for Solar-Driven H2O2 Production

Prasenjit Das; Gouri Chakraborty; Jérôme Roeser; Sarah Vogl; Jabor Rabeah; Arne Thomas

doi:10.1021/jacs.2c11454

Integrating Bifunctionality and Chemical Stability in Covalent Organic Frameworks via One-Pot Multicomponent Reactions for Solar-Driven H₂O₂ Production

J Am Chem Soc. 2023 Feb 8;145(5):2975-2984. doi: 10.1021/jacs.2c11454. Epub 2023 Jan 25.

Authors

Prasenjit Das¹, Gouri Chakraborty², Jérôme Roeser¹, Sarah Vogl¹, Jabor Rabeah³, Arne Thomas¹

Affiliations

¹ Department of Chemistry/Functional Materials, Technische Universität Berlin, 10623 Berlin, Germany.
² BAM Federal Institute for Materials Research and Testing, Richard-Willstätter-Str. 11, 12489 Berlin, Germany.
³ Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert-Einstein-Str. 29a, 18059 Rostock, Germany.

PMID: 36695541
DOI: 10.1021/jacs.2c11454

Abstract

Multicomponent reactions (MCRs) can be used to introduce different functionalities into highly stable covalent organic frameworks (COFs). In this work, the irreversible three-component Doebner reaction is utilized to synthesize four chemically stable quinoline-4-carboxylic acid DMCR-COFs (DMCR-1-3 and DMCR-1NH) equipped with an acid-base bifunctionality. These DMCR-COFs show superior photocatalytic H₂O₂ evolution (one of the most important industrial oxidants) compared to the imine COF analogue (Imine-1). This is achieved with sacrificial oxidants but also in pure water and under an oxygen or air atmosphere. Furthermore, the DMCR-COFs show high photostability, durability, and recyclability. MCR-COFs thus provide a viable materials' platform for solar to chemical energy conversion.