Asymmetric structure engineering of polymeric carbon nitride for visible-light-driven reduction reactions

• DOI: 10.1016/j.nanoen.2021.106168
• Publication Date: 2021-05-26T02:20:35Z
• Authors: Wei Luo; Yongli Li; Jinshu Wang; Jingchao Liu; Nan Zhang; Mengdi Zhao; Junshu Wu; Wenyuan Zhou; Lianzhou Wang
• Keywords: Carbon nitride; Ethylene diamine; Visible spectrum; Carbon fibers

Abstract The photocatalytic activity of polymeric carbon nitride (g-C3N4) strongly depends on its electronic structure which is highly sensitive to the preparation methods. To design the photocatalysts with efficient charge separation and transfer property, here we report a new ethylenediamine (EDA) induced gas-solid grafting method which enables the asymmetric modification of g-C3N4 featuring the aromatization at the terminal of melon motifs. The obtained terminal-aromatized g-C3N4 (Ar-C3N4) exhibits an improved visible-light-driven photocatalytic activity in versatile two-electron reduction reactions, outperforming the pristine g-C3N4 by 15.4 and 6.6 folds respectively in hydrogen evolution and hydrogen peroxide production. Theoretical and experimental results demonstrate the intensified asymmetry of π-electron distribution in the resulting material, which provides significantly improved driving force to guide the efficient separation of photogenerated e-h pairs and enhance the charge carrier mobility compared to its symmetric counterpart.