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Halogenated metal–organic framework glasses and liquids

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dc.contributor.authorHou, JWen_AU
dc.contributor.authorGómez, MLRen_AU
dc.contributor.authorKrajnc, Aen_AU
dc.contributor.authorMcCaul, Aen_AU
dc.contributor.authorLi, SSen_AU
dc.contributor.authorBumstead, AMen_AU
dc.contributor.authorSapnik, AFen_AU
dc.contributor.authorDeng, ZYen_AU
dc.contributor.authorLin, Ren_AU
dc.contributor.authorChater, PAen_AU
dc.contributor.authorKeeble, DSen_AU
dc.contributor.authorKeen, DAen_AU
dc.contributor.authorAppadoo, DRTen_AU
dc.contributor.authorChan, Ben_AU
dc.contributor.authorChen, Ven_AU
dc.contributor.authorMali, Gen_AU
dc.contributor.authorBennett, TDen_AU
dc.date.accessioned2026-07-23T00:52:17Zen_AU
dc.date.issued2020-01-24en_AU
dc.date.statistics2025-10-28en_AU
dc.description.abstractThe synthesis of four novel crystalline zeolitic imidazolate framework (ZIF) structures using a mixed-ligand approach is reported. The inclusion of both imidazolate and halogenated benzimidazolate-derived linkers leads to glass-forming behavior by all four structures. Melting temperatures are observed to depend on both electronic and steric effects. Solid-state NMR and terahertz (THz)/far-IR demonstrate the presence of a Zn-F bond for fluorinated ZIF glasses. In situ THz/far-IR spectroscopic techniques reveal the dynamic structural properties of crystal, glass, and liquid phases of the halogenated ZIFs, linking the melting behavior of ZIFs to the propensity of the ZnN4 tetrahedra to undergo thermally induced deformation. The inclusion of halogenated ligands within metal-organic framework (MOF) glasses improves their gas-uptake properties. © 2025 American Chemical Society.en_AU
dc.description.sponsorshipT.D.B. thanks the Royal Society for a University Research Fellowship (UF150021) and a research grant (RSG\R1\180395). J.H. and T.D.B also thank EPSRC (EP/R015481/1). J.H. thanks the Australian Research Council for a DECRA Fellowship (DE190100803). V.C. acknowledges financial support (DP180103874). S.L. acknowledges the China Scholarship Council (CSC). A.F.S. acknowledges the EPSRC for a Ph.D. studentship under the industrial CASE scheme along with Johnson Matthey PLC (JM11106). A.M.B. acknowledges the Royal Society for funding (RGF\EA\180092) as well as the Cambridge Trust for a Vice Chancellor’s Award (304253100). Z.D. thanks the Cambridge Trust and the China Scholarship Council. The calculations were performed at the U.K. National Supercomputing Service, ARCHER. Access was obtained via the UKCP consortium and funded by EPSRC under Grant no. EP/P022596/1. A.K. and G.M. acknowledge financial support from the Slovenian Research Agency (research core funding no. P1-0021 and research project Z1-9171). We thank U. Javornik for help with the liquid-state 19F NMR measurements. Generous computational resources are provided (to B.C.) by RIKEN Information Systems Division (Project Q19266). The authors acknowledge the facilities, and the scientific and technical assistance, of the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy and Microanalysis, The University of Queensland. Part of this research was undertaken on the THz/Far-IR beamline at the Australian Synchrotron, part of ANSTO (M14790 and EU15604). We acknowledge the provision of synchrotron access to Beamline I15-1 (EE20038-1 and EE20038-2) at the Diamond Light Source.en_AU
dc.format.mediumPrint-Electronicen_AU
dc.identifier.citationHou, J., Ríos Gómez, M. L., Krajnc, A., McCaul, A., Li, S., Bumstead, A. M., Sapnik, A. F., Deng, Z., Lin, R., Chater, P. A., Keeble, D. S., Keen, D. A., Appadoo, D., Chan, B., Chen, V., Mali, G., & Bennett, T. D. (2020). Halogenated metal–organic framework glasses and liquids. Journal of the American Chemical Society, 142(8), 3880–3890. doi:10.1021/jacs.9b11639en_AU
dc.identifier.issn0002-7863en_AU
dc.identifier.issn1520-5126en_AU
dc.identifier.issue8en_AU
dc.identifier.journaltitleJournal of the American Chemical Societyen_AU
dc.identifier.pagination3880-3890en_AU
dc.identifier.urihttps://doi.org/10.1021/jacs.9b11639en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/17277en_AU
dc.identifier.volume142en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectMetalsen_AU
dc.subjectMetallic glassesen_AU
dc.subjectLiquidsen_AU
dc.subjectZeolitesen_AU
dc.subjectLigandsen_AU
dc.subjectHalogenationen_AU
dc.subjectAmorphous stateen_AU
dc.subjectMeltingen_AU
dc.titleHalogenated metal–organic framework glasses and liquidsen_AU
dc.typeJournal Articleen_AU

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