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Instruments / Technical Area	Publication Details	Published
I15-1-X-ray Pair Distribution Function (XPDF)	Post-synthetic modification of a metal–organic framework glass Alice M. Bumstead , Ignas Pakamore , Kieran D. Richards , Michael F. Thorne , Sophia S. Boyadjieva , Celia Castillo-Blas , Lauren N. Mchugh , Adam F. Sapnik , Dean S. Keeble , David A. Keen , Rachel C. Evans , Ross S. Forgan , Thomas D. Bennett Chemistry Of Materials 28 DOI: 10.1021/acs.chemmater.1c03820 Diamond Proposal Number(s): [20038] Show Abstract ▼ Abstract: Melt-quenched metal–organic framework (MOF) glasses have gained significant interest as the first new category of glass reported in 50 years. In this work, an amine-functionalized zeolitic imidazolate framework (ZIF), denoted ZIF-UC-6, was prepared and demonstrated to undergo both melting and glass formation. The presence of an amine group resulted in a lower melting temperature compared to other ZIFs, while also allowing material properties to be tuned by post-synthetic modification (PSM). As a prototypical example, the ZIF glass surface was functionalized with octyl isocyanate, changing its behavior from hydrophilic to hydrophobic. PSM therefore provides a promising strategy for tuning the surface properties of MOF glasses.	Feb 2022
I15-1-X-ray Pair Distribution Function (XPDF)	Principles of melting in hybrid organic-inorganic perovskite and polymorphic ABX3 structures Bikash Kumar Shaw , Thomas D. Bennett , Celia Castillo-Blas , Michael F. Thorne , María Laura Ríos Gómez , Thomas Forrest , David A. Keen , Maria Diaz-Lopez , Philip A. Chater , Lauren N. Mchugh Chemical Science DOI: 10.1039/D1SC07080K Diamond Proposal Number(s): [20038] Open Access Show Abstract ▼ Abstract: Four novel dicyanamide-containing hybrid organic-inorganic ABX3 structures are reported, and the thermal behaviour of a series of nine perovskite and non-perovskite [AB(N(CN)2)3] (A = (C3H7)4N, (C4H9)4N, (C5H11)4N; B = Co, Fe, Mn). Structure-property relationships are investigated by varying both A-site organic and B-site transition metal cations. In particular, increasing the size of the A-site cation from (C3H7)4N → (C4H9)4N → (C5H11)4N was observed to result in a decrease in Tm through an increase in ΔSf. Consistent trends in Tm with metal replacement are observed with each A-site cation, with Co < Fe < Mn. The majority of the melts formed were found to recrystallise partially upon cooling, though glasses could be formed through a small degree of organic linker decomposition. Total scattering methods are used to provide a greater understanding of the melting mechanism	Jan 2022
I15-1-X-ray Pair Distribution Function (XPDF)	Glassy behaviour of mechanically amorphised ZIF-62 isomorphs Michael F. Thorne , Adam F. Sapnik , Lauren N. Mchugh , Alice M. Bumstead , Celia Castillo-Blas , Dean S. Keeble , Maria Diaz-Lopez , Philip A. Chater , David A. Keen , Thomas D. Bennett Chemical Communications DOI: 10.1039/D1CC03469C Diamond Proposal Number(s): [20038] Open Access Show Abstract ▼ Abstract: Zeolitic imidazolate frameworks (ZIFs) can be melt-quenched to form glasses. Here, we present an alternative route to glassy ZIFs via mechanically induced amorphisation. This approach allows various glassy ZIFs to be produced in under 30 minutes at room temperature, without the need for melt-quenching.	Aug 2021

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