A Data-Driven Search of Two-Dimensional Covalent Organic Frameworks for Visible-Light-Driven Overall Water Splitting

Two-dimensional (2D) covalent organic frameworks (COFs) with versatile structural and optoelectronic properties that can be tuned with building blocks and topological structures have received widespread attention for photocatalytic water splitting in recent years. However, few of these have been reported for overall water splitting under visible light. Here, we present a data-driven search of 2D COFs capable of visible-light-driven overall water splitting by combining high-throughput first-principles computations and experimental validations. Seven 2D COFs were identified to be capable of overall water splitting from the CoRE COF database, and their photocatalytic activities were further verified and optimized by our preliminary experiments. The production rates of H2 and O2 reached 80 and 32 μmol g-1 h-1, respectively, without using sacrificial agents. This work represents an attempt to explore 2D COFs for visible-light-driven overall water splitting with a data-driven approach that could accelerate the discovery and design of COFs toward photocatalytic overall water splitting.