In search of Covalent Organic Frameworkphotocatalysts: A DFT-based screening approach

Covalent organic frameworks (COFs) stand out as prospective organic-based photocatalysts given their intriguing optoelectronic properties, such as visible light absorption and high charge-carrier mobility. The CURATED COFs is a database of reported experimental COFs that until now remained mostly unexplored for photocatalysis. In this work, we screen the CURATED COFs database for discovering potential photocatalysts using a set of DFT-based descriptors that cost-effectively assesses visible light absorption, preliminary thermodynamic feasibility of the desired pair of redox reactions, charge separation, and charge-carrier mobility. The workflow can shortlist 13 COFs as prospective candidates for water splitting, and identify materials (Nx-COF, x=0-3) that have been reported as candidates for Hydrogen evolution reaction (HER). Overall, our strategy tackles the challenge of having too many COFs to explore by channeling the focus of future research to a selective group of COFs while elucidating insights into the structure design for a desired photocatalytic process.