Bottom-up design of 2D organic photocatalysts for visible-light driven hydrogen evolution

To design two-dimensional (2D) organocatalysts, three series of covalent organic frameworks (COFs) are constructed using bottom-up strategies, i.e. molecular selection, tunable linkage, and functionalization. First-principles calculations are performed to confirm their photocatalytic activity under visible light. Two of our constructed 2D COF models (B1 and C3) are identified as a sufficiently efficient organocatalyst for visible light water splitting. The controllable construction of such COFs from suitable organic subunit, linkage, and functional groups paves the way for correlating band edge alignments and geometry parameters of 2D organic materials. Our theoretical prediction not only provides essential insights into designing 2D-COF photocatalysts for water splitting, but also sparks other technological applications for 2D organic materials.