ORCID Profile
0000-0003-3842-3239
Current Organisation
University of St Andrews
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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: Wiley
Date: 21-02-2023
Abstract: Metal coordination compound (MCC) glasses [e.g., metal‐organic framework (MOF) glass, coordination polymer glass, and metal inorganic‐organic complex (MIOC) glass] are emerging members of the hybrid glass family. So far, a limited number of crystalline MCCs can be converted into glasses by melt‐quenching. Here, we report a universal wet‐chemistry method, by which the super‐sized supramolecular MIOC glasses can be synthesized from non‐meltable MOFs. Alcohol and acid were used as agents to inhibit crystallization. The MIOC glasses demonstrate unique features including high transparency, shaping capability, and anisotropic network. Directional photoluminescence with a large polarization ratio (≈47 %) was observed from s les doped with organic dyes. This crystallization‐suppressing approach enables fabrication of super‐sized MCC glasses, which cannot be achieved by conventional vitrification methods, and thus allows for exploring new MCC glasses possessing photonic functionalities.
Publisher: Royal Society of Chemistry (RSC)
Date: 17-09-2014
DOI: 10.1039/C4CP03298E
Abstract: An experimental study of Xe and Kr adsorption in metal-organic frameworks CPO-27-Ni, CPO-27-Mg, and ZIF-8 was carried out. In situ synchrotron X-ray powder diffraction experiments allowed precise determination of the adsorption sites and sequence of their filling with increasing of gas pressure at different temperatures. Structural investigations were used for interpretation of gas adsorption measurements.
Publisher: Wiley
Date: 07-12-2018
Publisher: Elsevier BV
Date: 09-2022
Publisher: Elsevier BV
Date: 2023
Publisher: Copernicus GmbH
Date: 27-03-2022
DOI: 10.5194/EGUSPHERE-EGU22-5818
Abstract: & & Catastrophic failure in brittle, porous materials initiates when structural damage, in the form of smaller-scale fractures, localises along an emergent failure plane or 'fault' in a transition from stable crack growth to dynamic rupture. Due to the extremely rapid nature of this critical transition, the precise micro-mechanisms involved are poorly understood and difficult to capture. However, these mechanisms are crucial drivers for devastating phenomena such as earthquakes, including induced seismicity, landslides and volcanic eruptions, as well as large-scale infrastructure collapse. Here we observe these micro-mechanisms directly by controlling the rate of micro-fracturing events to slow down the transition in a unique triaxial deformation experiment that combines acoustic monitoring with contemporaneous & em& in-situ& /em& x-ray imaging of the microstructure. The results provide the first integrated picture of how damage and associated micro-seismic events emerge and evolve together during localisation and failure and allow us to ground truth some previous inferences from mechanical and seismic monitoring alone. They also highlight where such inferences miss important kinematically-governed grain-scale mechanisms prior to and during shear failure.& & & & The evolving damage imaged in the 3D x-ray volumes and local strain fields undergoes a breakdown sequence involving several stages: (i) self-organised exploration of candidate shear zones close to peak stress, (ii) spontaneous tensile failure of in idual grains due to point loading and pore-emanating fractures within an emergent and localised shear zone, validating many inferences from acoustic emissions monitoring, and (iii) formation of a proto-cataclasite due to grain rotation and fragmentation, highlighting both the control of grain size on failure and the relative importance of aseismic mechanisms such as crack rotation in accommodating bulk shear deformation. Dilation and shear strain remain strongly correlated both spatially and temporally throughout s le weakening, confirming the existence of a cohesive zone, but with crack damage distributed throughout the shear zone rather than concentrated solely in a breakdown zone at the propagating front of a pre-existing discontinuity.& & & & Contrary to common assumption, we find seismic litude is not correlated with local imaged strain large local strain often occurs with small acoustic emissions, and vice versa. The seismic strain partition coefficient is very low overall and locally highly variable. Local strain is therefore predominantly aseismic, explained in part by grain/crack rotation along the emergent shear zone. The shear fracture energy calculated from local dilation and shear strain on the fault is half of that inferred from the bulk deformation, with a smaller critical slip distance, indicating that less energy is required for local breakdown in the shear zone compared with models of uniform slip.& & & & This improvement in process-based understanding holds out the prospect of reducing systematic errors in forecasting system-sized catastrophic failure in a variety of applications.& &
Publisher: Copernicus GmbH
Date: 15-05-2023
DOI: 10.5194/EGUSPHERE-EGU23-7933
Abstract: Catastrophic failure in brittle, porous materials initiates when structural damage, in the form of smaller-scale fractures, localises along an emergent failure plane or 'fault' in a transition from stable crack growth to dynamic rupture. Due to the extremely rapid nature of this critical transition, the precise micro-mechanisms involved are poorly understood and difficult to capture. However, these mechanisms are crucial drivers for devastating phenomena such as earthquakes, including induced seismicity, landslides and volcanic eruptions, as well as large-scale infrastructure collapse. Here we observe these micro-mechanisms directly by controlling the rate of micro-fracturing events to slow down the transition in a unique triaxial deformation experiment that combines acoustic monitoring with contemporaneous in-situ x-ray imaging of the microstructure. The results [1] provide the first integrated picture of how damage and associated micro-seismic events emerge and evolve together during localisation and failure and allow us to ground truth some previous inferences from mechanical and seismic monitoring alone. They also highlight where such inferences miss important kinematically-governed grain-scale mechanisms prior to and during shear failure.The evolving damage imaged in the 3D x-ray volumes and local strain fields undergoes a breakdown sequence involving several stages: (i) self-organised exploration of candidate shear zones close to peak stress, (ii) spontaneous tensile failure of in idual grains due to point loading and pore-emanating fractures within an emergent and localised shear zone, validating many inferences from acoustic emissions monitoring, (iii) formation of a proto-cataclasite due to grain rotation and fragmentation, highlighting both the control of grain size on failure and the relative importance of aseismic mechanisms such as crack rotation in accommodating bulk shear deformation. Dilation and shear strain remain strongly correlated both spatially and temporally throughout s le weakening, confirming the existence of a cohesive zone, but with crack damage distributed throughout the shear zone rather than concentrated solely in a breakdown zone at the propagating front of a pre-existing discontinuity.Contrary to common assumption, we find seismic litude is not correlated with local imaged strain large local strain often occurs with small acoustic emissions, and vice versa. The seismic strain partition coefficient is very low overall and locally highly variable. Local strain is therefore predominantly aseismic, explained in part by grain/crack rotation along the emergent shear zone. The shear fracture energy calculated from local dilation and shear strain on the fault is half of that inferred from the bulk deformation, with a smaller critical slip distance, indicating that less energy is required for local breakdown in the shear zone compared with models of uniform slip.This improvement in process-based understanding holds out the prospect of reducing systematic errors in forecasting system-sized catastrophic failure in a variety of applications.[1] Cartwright-Taylor et al. 2022, Nature Communications 13, 6169, 0.1038/s41467-022-33855-z
Publisher: Wiley
Date: 21-02-2023
Abstract: Metal coordination compound (MCC) glasses [e.g., metal‐organic framework (MOF) glass, coordination polymer glass, and metal inorganic‐organic complex (MIOC) glass] are emerging members of the hybrid glass family. So far, a limited number of crystalline MCCs can be converted into glasses by melt‐quenching. Here, we report a universal wet‐chemistry method, by which the super‐sized supramolecular MIOC glasses can be synthesized from non‐meltable MOFs. Alcohol and acid were used as agents to inhibit crystallization. The MIOC glasses demonstrate unique features including high transparency, shaping capability, and anisotropic network. Directional photoluminescence with a large polarization ratio (≈47 %) was observed from s les doped with organic dyes. This crystallization‐suppressing approach enables fabrication of super‐sized MCC glasses, which cannot be achieved by conventional vitrification methods, and thus allows for exploring new MCC glasses possessing photonic functionalities.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CP03304F
Abstract: Ion self-diffusion coefficients in ionic liquid solutions follow the Ertl–Dullien free volume power law with concentration dependent offsets.
Publisher: American Chemical Society (ACS)
Date: 05-04-2017
DOI: 10.1021/JACS.7B00106
Publisher: American Chemical Society (ACS)
Date: 13-06-2017
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Oxana V. Magdysyuk.