In Search of Covalent Organic Framework Photocatalysts: A DFT‐Based Screening Approach

Abstract 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 “Clean, Uniform, Refined with Automatic Tracking from Experimental Database” (CURATED) COFs is a database of reported experimental COFs that until now remained mostly unexplored for photocatalysis. In this study, the CURATED COFs database is screened 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 (N x ‐COF ( x = 0–3)) that have been reported as candidates for hydrogen evolution reaction. Overall, the strategy addresses the challenge of exploring a large number of COFs by directing future research toward a selective group of COFs, while providing valuable insights into the structural design for achieving a desired photocatalytic process.