Phosphorylation promotes liquid-phase proton transfer and carrier separation for boosted photocatalytic hydrogen evolution over g-C3N4

Abstract

Promoting liquid-phase proton transfer is crucial for enhancing photocatalytic hydrogen production reactions. However, existing research often overlooks this and focuses more on the study of the photocatalyst itself. In this paper, phosphorylation modification for enhancing photocatalytic hydrogen evolution activity of g-C₃N₄ (CN) via improving the proton transfer and carrier separation is explored. Experimental results and density functional theory (DFT) calculations reveal that the surface modification of CN with [aminotris(methylenephosphonic acid] (ATMP) can extend the response to visible light, promote the separation of photo-generated charge carriers and improve the transport of protons to reactive sites through constructing the solid–liquid contact interface on the surface of CN as well as regulating the physicochemical properties of both the solution interface and the CN itself, which therefore enhances the photocatalytic hydrogen evolution performance. This research offers a new strategy for the enhancement of the kinetics of photocatalytic hydrogen production by modifying the catalyst and tuning its “exterior surface” simultaneously.