In Search of Covalent Organic Framework Photocatalysts: 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 "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.