Browsing by Author "Macreadie LK"

Now showing 1 - 3 of 3
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    Gas adsorption in the topologically disordered Fe-BTC framework
    (Royal Society of Chemistry, 2021-11-19) Sapnik AF; Ashling CW; Macreadie LK; Lee SJ; Johnson T; Telfer SG; Bennett TD
    Disordered metal-organic frameworks are emerging as an attractive class of functional materials, however their applications in gas storage and separation have yet to be fully explored. Here, we investigate gas adsorption in the topologically disordered Fe-BTC framework and its crystalline counterpart, MIL-100. Despite their similar chemistry and local structure, they exhibit very different sorption behaviour towards a range gases. Virial analysis reveals that Fe-BTC has enhanced interaction strength with guest molecules compared to MIL-100. Most notably, we observe striking discrimination between the adsorption of C3H6 and C3H8 in Fe-BTC, with over a twofold increase in the amount of C3H6 being adsorbed than C3H8. Thermodynamic selectivity towards a range of industrially relevant binary mixtures is probed using ideal adsorbed solution theory. Together, this suggests the disordered material may possess powerful separation capabilities that are rare even amongst crystalline frameworks.
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    Guest size limitation in metal-organic framework crystal-glass composites
    (Royal Society of Chemistry, 2021-03-01) Ashling CW; Macreadie LK; Southern TJF; Zhang Y; McHugh LN; Evans RC; Kaskel S; Telfer SG; Bennett TD
    Metal-organic framework crystal-glass composites (MOF CGCs) have previously been formed by embedding crystalline MIL-53(Al) within a ZIF-62 glass (agZIF-62) matrix. Here we highlight thermal stability considerations in the formation of MOF CGCs, and subsequently report the synthesis of two novel MOF CGCs, by incorporating MIL-118 and UL-MOF-1 withinagZIF-62. These new materials, alongside the prototypical MOF CGC, formed using MIL-53(Al), were studied using scanning electron microscopy, powder X-ray diffraction, and gas sorption techniques. The gas uptake in composites formed from MIL-118C and UL-MOF-1 is largely dominated by theagZIF-62 matrix, suggesting that to improve the porosity of the MOF CGC, the matrix porosity must be improved, or a percolation threshold must be overcome.
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    In Situ Investigation of Multicomponent MOF Crystallization during Rapid Continuous Flow Synthesis
    (American Chemical Society, 2021-11-17) He B; Macreadie LK; Gardiner J; Telfer SG; Hill MR
    Access to the potential applications of metal-organic frameworks (MOFs) depends on rapid fabrication. While there have been advances in the large-scale production of single-component MOFs, rapid synthesis of multicomponent MOFs presents greater challenges. Multicomponent systems subjected to rapid synthesis conditions have the opportunity to form separate kinetic phases that are each built up using just one linker. We sought to investigate whether continuous flow chemistry could be adapted to the rapid formation of multicomponent MOFs, exploring the UMCM-1 and MUF-77 series. Surprisingly, phase pure, highly crystalline multicomponent materials emerge under these conditions. To explore this, in situ WAXS was undertaken to gain an understanding of the formation mechanisms at play during flow synthesis. Key differences were found between the ternary UMCM-1 and the quaternary MUF-7, and key details about how the MOFs form were then uncovered. Counterintuitively, despite consisting of just two ligands UMCM-1 proceeds via MOF-5, whereas MUF-7 consists of three ligands but is generated directly from the reaction mixture. By taking advantage of the scalable high-quality materials produced, C6 separations were achieved in breakthrough settings.