“…[33][34][35] Among various 2D nanomaterials, graphitic carbon nitride (g-C 3 N 4 ) has been regarded as an excellent substrate for supporting metal-based catalysts, because it contains intrinsic evenly distributed holes surrounded by electron-rich N atoms, which can provide abundant electron lone pairs for anchoring metal ions within its ligands. [36][37][38][39][40][41][42] In particular, g-C 3 N 4 could act as a molecular scaffold for appropriately tuning the electronic properties of the anchored metal centers to endow them with high catalytic activity and selectivity in electrocatalysis. [43][44][45] Motivated by the aforementioned studies, taking the widely investigated Cu as a module, we investigated the catalytic performance of several sub-nano Cu n (n ¼ 1-6) clusters supported by g-C 3 N 4 (Cu n @g-C 3 N 4 ) as COER catalysts by means of density functional theory (DFT) computations.…”