Next, we used density functional theory (DFT) calculations to better understand the origin of paramagnetism in the NiPACN materials. We used two distinct NiN4C8 and NiN4C10 model structures to represent the dispersed NiNx CO2R active sites. In the NiN4C8 model, the NiN4 moiety acts as a bridge between two adjacent armchair edges of graphene allowing NiN4 to be tetrahedrally distorted (D2d symmetry), creating two intersecting planes under a dihedral angle between 180° and 90° (Figure and SI-Figure ). For the NiN4C10 model, we studied both non-periodic and periodic configurations, where the square-planar (D4h symmetry) NiN4 moiety is embedded on a flat graphite layer (SI-Figure ).