ORCID Profile
0000-0001-9231-3749
Current Organisation
University of Oxford
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Publisher: Wiley
Date: 07-12-2018
Abstract: There is an increasing amount of interest in metal-organic frameworks (MOFs) for a variety of applications, from gas sensing and separations to electronics and catalysis. However, the mechanisms by which they crystallize remain poorly understood. Herein, an important new insight into MOF formation is reported. It is shown that, prior to network assembly, crystallization intermediates in the canonical ZIF-8 system exist in a dynamic pre-equilibrium, which depends on the reactant concentrations and the progress of reaction. Concentration can, therefore, be used as a synthetic handle to directly control particle size, with potential implications for industrial scale-up and gas sorption applications. These findings enable the rationalization of apparent contradictions between previous studies of ZIF-8 and opens up new opportunities for the control of crystallization in network solids more generally.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 27-01-2023
Abstract: When tiles decorated to lower their symmetry are joined together, they can form aperiodic and labyrinthine patterns. Such Truchet tilings offer an efficient mechanism of visual data storage related to that used in barcodes and QR codes. We show that the crystalline metal–organic framework [OZn 4 ][1,3-benzenedicarboxylate] 3 (TRUMOF-1) is an atomic-scale realization of a complex three-dimensional Truchet tiling. Its crystal structure consists of a periodically arranged assembly of identical zinc-containing clusters connected uniformly in a well-defined but disordered fashion to give a topologically aperiodic microporous network. We suggest that this unusual structure emerges as a consequence of geometric frustration in the chemical building units from which it is assembled.
Publisher: Springer Science and Business Media LLC
Date: 27-05-2021
DOI: 10.1038/S41557-021-00684-4
Abstract: The ultrahigh porosity and varied functionalities of porous metal-organic frameworks make them excellent candidates for applications that range widely from gas storage and separation to catalysis and sensing. An interesting feature of some frameworks is the ability to open their pores to a specific guest, enabling highly selective separation. A prerequisite for this is bistability of the host structure, which enables the framework to breathe, that is, to switch between two stability minima in response to its environment. Here we describe a porous framework DUT-8(Ni)-which consists of nickel paddle wheel clusters and carboxylate linkers-that adopts a configurationally degenerate family of disordered states in the presence of specific guests. This disorder originates from the nonlinear linkers arranging the clusters in closed loops of different local symmetries that in turn propagate as complex tilings. Solvent exchange stimulates the formation of distinct disordered frameworks, as demonstrated by high-resolution transmission electron microscopy and diffraction techniques. Guest exchange was shown to stimulate repeatable switching transitions between distinct disorder states.
Publisher: Wiley
Date: 07-12-2018
Publisher: Springer Science and Business Media LLC
Date: 15-04-2021
DOI: 10.1038/S41467-021-22515-3
Abstract: Spin-ices are frustrated magnets that support a particularly rich variety of emergent physics. Typically, it is the interplay of magnetic dipole interactions, spin anisotropy, and geometric frustration on the pyrochlore lattice that drives spin-ice formation. The relevant physics occurs at temperatures commensurate with the magnetic interaction strength, which for most systems is 1–5 K. Here, we show that non-magnetic cadmium cyanide, Cd(CN) 2 , exhibits analogous behaviour to magnetic spin-ices, but does so on a temperature scale that is nearly two orders of magnitude greater. The electric dipole moments of cyanide ions in Cd(CN) 2 assume the role of magnetic pseudospins, with the difference in energy scale reflecting the increased strength of electric vs magnetic dipolar interactions. As a result, spin-ice physics influences the structural behaviour of Cd(CN) 2 even at room temperature.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8DT01128A
Abstract: We report the nonaqueous synthesis of Cd(CN) 2 by oxidation of cadmium metal with Hg(CN) 2 in liquid ammonia.
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Andrew Goodwin.