We first analyze the synthesized ZIF-4-bImCl, ZIF-62-bImCl, and ZIF-8-bImCl samples (with varying R) using FTIR and Raman spectroscopy, revealing that the imidazolate and benzimidazolate linkers remain intact and do not decompose upon melt-quenching (Supplementary Figs. , Supplementary Table , Supplementary Text). We also probe the structure of the modified ZIF glasses (for R=1.0 using bImCl) through X-ray photoelectron spectroscopy (XPS, see Supplementary Figs. 13-14) and compare the spectra to those of the unmodified ZIF crystals (noting that the XPS signal of ZIF glasses and crystals are known to be very similar ). Upon glass formation, we observe a broadening of the C1s, N1s, and Zn2p peaks as well as an additional shoulder peak in the N1s spectra for all glasses at relatively high energy (~404 eV). We assign the latter to the formation of pyrrolic nitrogen (N bonded to both C and H) upon co-melting with the halide salt, as this species is introduced through the bIm + cation in contrast to the lower-energy peak (~402 eV) from pyridinic nitrogen (N bonded to C).