Hybrid glasses from strong and fragile metal-organic framework liquids

Thomas D. Bennett (), Jin-Chong Tan, Yuanzheng Yue, Emma Baxter, Caterina Ducati, Nick J. Terrill, Hamish H. -M. Yeung, Zhongfu Zhou, Wenlin Chen, Sebastian Henke, Anthony K. Cheetham and G. Neville Greaves ()
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Thomas D. Bennett: University of Cambridge
Jin-Chong Tan: University of Oxford
Yuanzheng Yue: Section of Chemistry, Aalborg University
Emma Baxter: University of Cambridge
Caterina Ducati: University of Cambridge
Nick J. Terrill: Diamond Light Source Ltd, Diamond House, Harwell Science and Innovation Campus
Hamish H. -M. Yeung: International Center of Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS)
Zhongfu Zhou: Institute of Mathematics, Physics and Computer Science, Aberystwyth University
Wenlin Chen: Institute of Mathematics, Physics and Computer Science, Aberystwyth University
Sebastian Henke: University of Cambridge
Anthony K. Cheetham: University of Cambridge
G. Neville Greaves: University of Cambridge

Nature Communications, 2015, vol. 6, issue 1, 1-7

Abstract: Abstract Hybrid glasses connect the emerging field of metal-organic frameworks (MOFs) with the glass formation, amorphization and melting processes of these chemically versatile systems. Though inorganic zeolites collapse around the glass transition and melt at higher temperatures, the relationship between amorphization and melting has so far not been investigated. Here we show how heating MOFs of zeolitic topology first results in a low density ‘perfect’ glass, similar to those formed in ice, silicon and disaccharides. This order–order transition leads to a super-strong liquid of low fragility that dynamically controls collapse, before a subsequent order–disorder transition, which creates a more fragile high-density liquid. After crystallization to a dense phase, which can be remelted, subsequent quenching results in a bulk glass, virtually identical to the high-density phase. We provide evidence that the wide-ranging melting temperatures of zeolitic MOFs are related to their network topologies and opens up the possibility of ‘melt-casting’ MOF glasses.

Date: 2015
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DOI: 10.1038/ncomms9079

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