In conclusion, we arrive at a structural description of PTI-IF as a corrugated, and or AB stacked, intercalate-free, triazine-based material coming from various, orthogonal methods that encompass we propose dipolar interactions of adjacent PTI-layers due to the polar CN-bonds. Removal of the intercalated ions from PTI-LiBr has a pronounced effect on the local electronic environments of carbon-and nitrogen nuclei in PTI-IF that we monitored using solid-state NMR (ssNMR). Carbon environments attributed to the triazine (C3N3) ring are split up as C (168, 162, 157 ppm) in the PTI-LiBr structure by the heterogenous distribution of intercalated ions. In comparison, the more homogeneous, intercalate-free PTI-IF structure shows only one carbon signal at 163 ppm (Figure ). Similarly, the N signals of PTI-IF appear sharper at -179 (triazine nitrogens) and -255 ppm (imide bridge nitrogen) (Figure ).