Nitrogen-rich carbon nitride (C3N5) coupled with oxygen vacancy TiO2 arrays for efficient photocatalytic H2O2 production

J Colloid Interface Sci. 2024 Jan;653(Pt B):1028-1039. doi: 10.1016/j.jcis.2023.09.136. Epub 2023 Sep 25.

Abstract

Developing efficient and facilitated recycling photocatalysts for H2O2 formation is an ideal strategy for solar-to-chemical energy conversion. In this work, we synthesized ultrathin C3N5 nanosheets through the process of thermal polymerization and polyvinylpyrrolidone (PVP)-assisted solvent exfoliation. Subsequently, the obtained ultrathin C3N5 nanosheets were tightly attached to the surface of TiO2-x arrays, resulting in an enhanced photocatalytic H2O2 production rate. The density functional theory (DFT) calculations demonstrate that an internal electric field (IEF) is generated between the TiO2-x array and the ultrathin C3N5 due to the different work functions. The presence of IEF provides an additional driving force for carrier separation and transfer in the heterointerface. Benefitting from this unique strategy, the optimal heterojunction obtains the highest H2O2 formation rate (2.93 μmol/L/min), which is about 4.1 times than that of TiO2-x arrays. The rotating disk electrode (RDE) analysis manifests H2O2 formation through 2e--dominated oxygen reduction reaction (ORR). This research provides an innovative strategy for assembling a type-II heterojunction with a useful IEF for efficient photocatalytic H2O2 production.

Keywords: C(3)N(5) nanosheets; H(2)O(2) production; Oxygen vacancy TiO(2); Photocatalytic mechanism.