We then characterize the structure of the modified ZIF-62-bImCl (R=1.0) glass using high-field solid-state 67 Zn, 15 N, C, and 1 H magic-angle spinning (MAS) NMR spectroscopy and compare the results to those of the unmodified ZIF-62 glass . The 67 Zn MAS NMR data in Fig. (including a simulated spectrum made using SIMPSON ) show a slight change of the chemical shift upon comelting with the bImCl salt. In comparison to previous 67 Zn measurements of ZIF-62 glass (diso=278 ppm) and crystalline bis(imidazole)zinc(II) chloride (diso=265 ppm) 15 N MAS NMR shifts upon halide salt addition, including the appearance of multiple new peaks, which we assign to non-bridging benzimidazole and imidazole species as introduced from the bImCl salt and the network itself. This is because the two N are not equivalent in the modified ZIF glass structure as one is protonated (d<180 ppm) while the other is linked to Zn (d>180 ppm) (see sketches in Supplementary Figs. 15-17). Furthermore, the addition of benzimidazole species through the bImCl salt is clearly seen as an increase in the intensity at d~190 ppm (Supplementary Fig. ). Similarly, the solid-state C MAS NMR measurements show the enhanced intensity of peaks due to benzimidazole species in the structure (d~110-130 ppm region in Supplementary Fig. ). New peaks at d~135 ppm furthermore indicate the asymmetry of electron density associated with the pure Im and bIm species . The solid-state 1 H MAS NMR measurements reveal a broad peak around 5-7 ppm for both ZIF-62 and ZIF-62-bImCl glasses, which we assign to the aromatic proton. Finally, an additional peak at ~12 ppm is observed in the ZIF-62-bImCl glass (Supplementary Fig17), which we ascribe to the N-H proton in pure Im and bIm species 40 .