Improved charge transfer in polymeric carbon nitride synergistically induced by the aromatic rings modification and Schottky junctions for efficient photocatalytic CO2 reduction

Abstract

Polymeric carbon nitride (CN) is one of the most prospective non-metallic catalysts at present, yet its photocatalytic activity is unsatisfactory mainly due to the poor intramolecular charge carrier separation efficiency originated form its special electronic structure. Herein, we demonstrate a synergistic strategy to improve the charge carriers transfer and separation efficiency of CN synchronously by extending the π-conjugated system via incorporation of O-containing aromatic ring in the CN skeleton (Ar-CN) and constructing a Schottky junction via decoration of Au nanoparticles (Au Nps). The introduced O-containing aromatic ring can create a local asymmetry, delocalize the π-conjugated system of CN, and thus promote the in-plane charge transport of CN, while the formed loading of Au Nps can further promote interlayer charge transfer efficiency of Ar-CN. The optimized 3 %Au/Ar-CN photocatalyst exhibits a high photocatalytic CO2 activity with a CO yield of 32.03 μmol·g−1·h−1, which is higher than those of CN (2.38 μmol·g−1·h−1) and Ar-CN (6.42 μmol·g−1·h−1). This study provides a feasible co-modification strategy to enhance the charge transfer and photocatalytic activity of CN by extending the π-conjugation system and constructing Schottky junctions.