High-Throughput\nComputational Screening of Novel Two-Dimensional\nCovalent Organic Frameworks for Efficient Photocatalytic Overall Water\nSplitting

Abstract

The pursuit of efficient photocatalysts toward photocatalytic\nwater\nsplitting has attracted wide attention. However, the low efficiency\nof photocatalytic reactions due to the rapid electron–hole\nrecombination and the time-consuming searching process hinder the\ndevelopment of high-performance photocatalysts. Here, we proposed\na data-driven screening procedure for covalent organic frameworks\n(COFs) as overall solar water-splitting photocatalysts. Based on a\nCOF database through assembling different <i>Cores</i> and <i>Linkers</i>, three COFs are predicted to be efficient photocatalysts\nfor overall solar water splitting after high-throughput computational\nscreening. We found that the photogenerated electrons and holes are\nwell separated on single COF photocatalysts without material engineering,\nand both hydrogen and oxygen evolution reactions can occur spontaneously\non the three screened COFs under visible light radiation. This kind\nof novel COF screened by a data-driven screening procedure offers\nnew perspectives for advancing efficient photocatalysts.