Boosting Photocatalytic H₂O₂ Generation by Constructing a Cyano and Carbon Dots/Polypyrrole Co‐Modified Carbon Nitride Heterostructure

Abstract Constructing heterostructure is a promising strategy to enhance photocatalytic performance. Here, a cyano and carbon dots/polypyrrole (CDs/PPy) co‐modified carbon nitride (CPKCN) heterostructure is constructed for photocatalytic H₂O₂ generation. It is interestingly found that the intermediates formed during the oxidation polymerization of pyrrole can be the potential electron trapping sites and reactive sites. In addition, the localized photoheat produced by CDs/PPy also plays an active role in improving photocatalytic activity. Moreover, the addition of CDs/PPy leads to a higher negative zeta potential of CPKCN, which is favorable for the attraction of the sample surface to H⁺. These features, plus the positive effect of cyano groups, collectively boost the charge transfer and improve the selectivity of two‐electron O₂ reduction. Therefore, the enhanced photocatalytic H₂O₂ generation performance of the developed CPKCN is achieved, with an H₂O₂ generation rate of 3.7 mmol g⁻¹ h⁻¹ under visible light in a 10 vol% isopropanol (IPA) aqueous solution, and with the apparent quantum yield of 16.7% at 420 nm and the solar‐to‐chemical conversion efficiency of 0.34%. The work offers new insights into developing efficient photocatalysts for various applications.