Carbon nitride (C 3 N 4) comprises earth-abundant carbon and nitrogen elements and was first called "melon" by Liebig in 1834. A melon structure was proposed by Lotsch et al in 2007, 2 in which one-dimensional zigzag chains consisting of multiple planar frameworks (melem) were linked by hydrogen bonds with amine groups to form closely packed two-dimensional arrays. Thus, a melon structure is not fully condensed graphitic C 3 N 4. 3 As a metal-free polymeric semiconductor, low-cost C 3 N 4 is used because of its simple synthesis, visible-light response (~2.7 eV), nontoxicity, tunable textures and electronic structures, and excellent thermal and chemical stability. 4-10 Visible-light-driven photocatalytic water splitting, in which C 3 N 4 is applied to working electrodes in photoelectrochemical (PEC) cells, has been a promising application since its first study in 2009. 4,5,7-14 Photodegradation of soluble dyes 4,9,15 and air pollutants 9,16 has also been reported. Furthermore, density functional theory has been widely used to investigate C 3 N 4 as photocatalysts. 17 However, problems