Advanced Functional Carbon Nitride by Implanting Semi‐Isolated VO2 Active Sites for Photocatalytic H2 Production and Organic Pollutant Degradation

Abstract It is critical to facilitate surface interaction for liquid–solid two‐phase photocatalytic reactions. This study demonstrates more advanced, efficient, and rich molecular‐level active sites to extend the performance of carbon nitride (CN). To achieve this, semi‐isolated vanadium dioxide is obtained by controlling the growth of non‐crystalline VO 2 anchored into sixfold cavities of the CN lattice. As a proof‐of‐concept, the experimental and computational results solidly corroborate that this atomic‐level design has potentially taken full advantage of two worlds. The photocatalyst comprises the highest dispersion of catalytic sites with the lowest aggregation, like single‐atom catalysts. It also demonstrates accelerated charge transfer with the boosted electron–hole pairs, mimicking heterojunction photocatalysts. Density functional theory calculations show that single‐site VO 2 anchored into the sixfold cavities significantly elevates the Fermi level, compared with the typical heterojunction. The unique features of semi‐isolated sites result in a high visible‐light photocatalytic H 2 production of 645 µmol h −1 g −1 with only 1 wt% Pt. They also represent an excellent photocatalytic degradation for rhodamine B as well as tetracycline, surpassing the activities obtained from many conventional heterojunctions. This study presents exciting opportunities for the design of new heterogeneous metal oxide for a variety of reactions.