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Successful synthesis of the nitrogenated holey two-dimensional structures C2N(Nat. Commun. 2015, 6, 6486) using simply wet-chemical reaction offer acost-effective way to generate other 2D materials with novel optical andelectronic properties. On basis of the density functional theory calculations,we investigate electronic properties of monolayer and multilayer C2N. We findthat few-layer C2N have a direct bandgap and the direct bandgap of the systemcan vary from 2.47 eV for monolayer to 1.84 eV for a five-layer. Besides, forthe few-layer C2N, appropriate band gap, band edge alignments, and strongvisible-light absorption demonstrate it may be a potential metal-freevisible-light driven photocatalyst for water splitting.

Few-Layer C2N: A Promising Metal-free Photocatalyst for Water Splitting