Publications
92 results found
Podda E, Arca M, Pintus A, et al., 2023, On the role of torsional dynamics in the solid-state fluorescent properties of a new bifluorene-tetracarboxylic acid and its supramolecular assemblies: a structural and TD-DFT investigation, CrystEngComm, Vol: 25, Pages: 1058-1066, ISSN: 1466-8033
The novel butterfly-shaped tetracarboxylic acid [9,9'-methylene-bis(9-methylfluorene-2,7-dicarboxylic acid), H4L] featuring a co-facial bifluorene core was designed and synthesised. Reactions of H4L with CdII produced the luminescent supramolecular frameworks 2 and 3, with different dimensionality and wingspan of L4–. The solid-state emission properties were rationalised based on the torsional dynamics of the facing bifluorene units by means of X-ray diffraction analysis and DFT calculations.
Davies R, Ma X, 2022, Tartramide ligands for copper-catalyzed N-Arylation at room temperature, Advanced Synthesis and Catalysis, Vol: 364, ISSN: 1615-4150
Abstract. A novel class of readily accessible tartramide ligands has been demonstrated to promote copper-catalysed N-arylation under mild conditions. In addition, the coupling protocol employs cheap and readily available pre-catalyst, ligand, and base (NaOH), and overcomes many current limitations often associated with Ullmann coupling: it can be run with low catalyst loadings, does not require the use of excess amine, gives excellent conversions at room temperature, is fully homogeneous, and displays improved tolerance to air and moisture. Detailed kinetic studies using reaction progress kinetic analysis (RPKA) methods have provided insight into the factors influencing the reaction rate in terms of impact of ligand structure, reactant / catalyst dependence and catalyst (in)stability. These kinetic insights have been used in a quality-by-design approach for further optimization of the reaction protocol. The reaction scope was extended to 22 examples, showing broad applicability for a wide range of substituted aryl iodides with both primary and secondary amines.
Podda E, Coles SJ, Horton PN, et al., 2021, First example of solid-state luminescent borasiloxane-based chiral helices assembled through N-B bonds, DALTON TRANSACTIONS, Vol: 50, Pages: 3782-3785, ISSN: 1477-9226
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- Citations: 3
Mohamed NA, Abou-Saleh H, Kameno Y, et al., 2021, Studies on metal-organic framework (MOF) nanomedicine preparations of sildenafil for the future treatment of pulmonary arterial hypertension, Scientific Reports, Vol: 11, Pages: 1-8, ISSN: 2045-2322
Pulmonary arterial hypertension (PAH) is an incurable disease, although symptoms are treated with a range of dilator drugs. Despite their clinical benefits, these drugs are limited by systemic side-effects. It is, therefore, increasingly recognised that using controlled drug-release nanoformulation, with future modifications for targeted drug delivery, may overcome these limitations. This study presents the first evaluation of a promising nanoformulation (highly porous iron-based metal–organic framework (MOF); nanoMIL-89) as a carrier for the PAH-drug sildenafil, which we have previously shown to be relatively non-toxic in vitro and well-tolerated in vivo. In this study, nanoMIL-89 was prepared and charged with a payload of sildenafil (generating Sil@nanoMIL-89). Sildenafil release was measured by Enzyme-Linked Immunosorbent Assay (ELISA), and its effect on cell viability and dilator function in mouse aorta were assessed. Results showed that Sil@nanoMIL-89 released sildenafil over 6 h, followed by a more sustained release over 72 h. Sil@nanoMIL-89 showed no significant toxicity in human blood outgrowth endothelial cells for concentrations up to100µg/ml; however, it reduced the viability of the human pulmonary artery smooth muscle cells (HPASMCs) at concentrations > 3 µg/ml without inducing cellular cytotoxicity. Finally, Sil@nanoMIL-89 induced vasodilation of mouse aorta after a lag phase of 2–4 h. To our knowledge, this study represents the first demonstration of a novel nanoformulation displaying delayed drug release corresponding to vasodilator activity. Further pharmacological assessment of our nanoformulation, including in PAH models, is required and constitutes the subject of ongoing investigations.
Delmas LC, White AJP, Pugh D, et al., 2020, Stable metal-organic frameworks with low water affinity built from methyl-siloxane linkers, CHEMICAL COMMUNICATIONS, Vol: 56, Pages: 7905-7908, ISSN: 1359-7345
Al-Ansari DE, Mohamed NA, Marei I, et al., 2020, Internalization of Metal-Organic Framework Nanoparticles in Human Vascular Cells: Implications for Cardiovascular Disease Therapy, NANOMATERIALS, Vol: 10
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- Citations: 5
Mohamed NA, Davies RP, Lickiss PD, et al., 2019, Mil-89 nanoformulation as a platform to improve pulmonary arterial hypertension treatment, British-Pharmacology-Society Meeting (Pharmacology), Publisher: WILEY, Pages: 3075-3075, ISSN: 0007-1188
Lo Q, Sale D, Braddock D, et al., 2019, New insights into the reaction capabilities of ionic organic bases in cu-catalysed amination, European Journal of Organic Chemistry, Vol: 2019, Pages: 1944-1951, ISSN: 1099-0690
The application of ionic organic bases in the copper‐catalyzed amination reaction (Ullmann reaction) has been studied at room temperature, with sub‐mol‐% catalyst loadings, and with more challenging amines at elevated temperatures. The cation present in the base has been shown to have little effect on the reaction at standard catalyst and ancillary ligand loadings, whereas the choice of anion is crucial for good reactivity. A substrate scope carried out at room temperature with the best performing bases, TBAM and TBPM, showed both bases to be highly effective under these mild reaction conditions. Moreover, under sub‐mol % catalyst loadings and room temperature conditions, TBPM gave good to excellent yields for a number of different amines and functionalized aryl iodides (14 examples). However, reactions involving more challenging amines gave little or no yield. By using more forceful conditions (120 °C) moderate to excellent yields of cross‐coupled products containing more challenging amines was achievable using TBPM and to a lesser extent with TBAM. As part of this work a study on the stability of the organic bases at 120 °C was undertaken. TBAM is shown to decompose to give nBu3N and mono‐butylmalonate at higher temperatures, and this can be correlated to a decrease in performance in the coupling reaction. The phosphonium cations in TBPM did not undergo analogous reactivity but were shown instead to experience some degree of deprotonation at the α‐CH2 to generate phosphonium ylides. This however did not lead to a significantly degradation in the activity of the TBPM in the cross‐coupling reaction.
Pugh D, Ashworth E, Robertson K, et al., 2019, Metal-organic frameworks constructed from group 1 metals (Li, Na) and silicon-centered linkers, Crystal Growth and Design, Vol: 19, Pages: 487-497, ISSN: 1528-7483
A series of “light metal” metal–organic frameworks containing secondary building units (SBUs) based on Li+ and Na+ cations have been prepared using the silicon-centered linkers MexSi(p-C6H4CO2H)4-x (x = 2, 1, 0). The unipositive charge, small size, and oxophilic nature of the metal cations give rise to some unusual and unique SBUs, including a three-dimensional nodal structure built from sodium and oxygen ions when using the triacid linker (x = 1). The same linker with Li+ cations generated a chiral, helical SBU, formed from achiral starting materials. One-dimensional rod SBUs are observed for the diacid (x = 2) and tetra-acid (x = 0) linkers with both Li+ and Na+ cations, where the larger size of Na+ compared to Li+ leads to subtle differences in the constitution of the metal nodes.
Davies RP, Delmas L, Horton P, et al., 2019, Studies on the structural diversity of MOFs containing octahedral siloxane-backboned connectors, Polyhedron, Vol: 157, Pages: 25-32, ISSN: 0277-5387
Four metal–organic frameworks containing hexatopic connectors have been prepared and structurally characterised: [Cd3(L)(DMA)2(H2O)2] (IMP-28), [Ce2(L)(DMF)2(H2O)2] (IMP-29), [Y2(L)(DMF)2(H2O)2] (IMP-30), and [Zn2(L-H2)(4,4′-bipy)2] (IMP-31). All the MOFs have been constructed using the hybrid inorganic–organic siloxane linker hexakis(4-carboxyphenyl)disiloxane (L-H6). In each case, discrete metal-based nodes are cross-linked by the octahedrally disposed connector to afford 3D polymeric structures. The underlying nets in these MOFs have been evaluated through deconstruction of their crystal structures and subsequent topological analysis. Examples of MOFs built from hexatopic linkers, and especially those with octahedral predispositions such as in L, remain scarce and the topologies ascribed to some of these MOFs are unique.
Delmas L, White A, Pugh D, et al., 2018, Trisiloxane-centred metal-organic frameworks and hydrogen bonded assemblies, CrystEngComm, Vol: 20, Pages: 4541-4545, ISSN: 1466-8033
A hexacarboxylic acid with a trisiloxane backbone (L-H6) has been prepared and applied in MOF construction. L-H6 itself crystallizes as an unusual 2D hydrogen-bonded network. Reaction of L-H6 with Mn(II) gave IMP-20 and with Zn(II) gave IMP-21: both are 3D MOFs incorporating Si–O–Si–O–Si linkages.
Grigoropoulos A, McKay AI, Katsoulidis AP, et al., 2018, Encapsulation of Crabtree's Catalyst in Sulfonated MIL‐101(Cr): Enhancement of Stability and Selectivity between Competing Reaction Pathways by the MOF Chemical Microenvironment, Angewandte Chemie, Vol: 130, Pages: 4622-4627, ISSN: 0044-8249
Grigoropoulos A, McKay AI, Katsoulidis AP, et al., 2018, Encapsulation of Crabtree's catalyst in sulfonated MIL-101(Cr): enhancement of stability and selectivity between competing reaction pathways by the MOF chemical microenvironment, Angewandte Chemie International Edition, Vol: 57, Pages: 4532-4537, ISSN: 1521-3757
Crabtree's catalyst was encapsulated inside the pores of the sulfonated MIL-101(Cr) metal-organic framework (MOF) by cation exchange. This hybrid catalyst is active for the heterogeneous hydrogenation of non-functionalized alkenes either in solution or in the gas phase. Moreover, encapsulation inside a well-defined hydrophilic microenvironment enhances catalyst stability and selectivity to hydrogenation over isomerization for substrates bearing ligating functionalities. Accordingly, the encapsulated catalyst significantly outperforms its homogeneous counterpart in the hydrogenation of olefinic alcohols in terms of overall conversion and selectivity, with the chemical microenvironment of the MOF host favouring one out of two competing reaction pathways.
Lo QA, Sale D, Braddock DC, et al., 2017, Mechanistic and Performance Studies on the Ligand Promoted Ullmann Amination Reaction, ACS Catalysis, Vol: 8, Pages: 101-109, ISSN: 2155-5435
Over the last two decades many different auxiliary ligand systems have been utilized in the copper-catalyzed Ullmann amination reaction. However, there has been little consensus on the relative merits of the varied ligands and the exact role they might play in the catalytic process. Accordingly, in this work some of the most commonly employed auxiliary ligands have been evaluated for C–N coupling using reaction progress kinetic analysis (RPKA) methodology. The results reveal not only the relative kinetic competencies of the different auxiliary ligands but also their markedly different influences on catalyst degradation rates. For the model Ullmann reaction between piperidine and iodobenzene using the soluble organic base bis(tetra-n-butylphosphonium) malonate (TBPM) at room temperature, N-methylglycine was shown to give the best performance in terms of high catalytic rate of reaction and comparatively low catalyst deactivation rates. Further experimental and rate data indicate a common catalytic cycle for all auxiliary ligands studied, although additional off-cycle processes are observed for some of the ligands (notably phenanthroline). The ability of the auxiliary ligand, base (malonate dianion), and substrate (amine) to all act competitively as ligands for the copper center is also demonstrated. On the basis of these results an improved protocol for room-temperature copper-catalyzed C–N couplings is presented with 27 different examples reported.
Davies RP, Delmas L, Horton PN, et al., 2017, Siloxane-based linkers in the construction of hydrogen bonded assemblies and porous 3D MOFs, Chemical Communications, Vol: 53, Pages: 12524-12527, ISSN: 1359-7345
A siloxane-based hexacarboxylic acid (L1-H6) has been prepared and applied in MOF construction. L1-H6 itself crystallizes as an unusual interpenetrated 3D hydrogen-bonded framework. Reaction of L1-H6 with Zn(II) gave IMP-18 – a 3D MOF incorporating Si–O–Si functionality. Cleavage of L1-H6 gives a silanol-based triacid which is shown to give a coordination polymer (IMP-19) with Zn(II).
Mohamed NA, Davies RP, Lickiss PD, et al., 2017, Chemical and biological assessment of metal organic frameworks (MOFs) in pulmonary cells and in an acute in vivo model: relevance to pulmonary arterial hypertension therapy, Pulmonary Circulation, Vol: 7, Pages: 1-11, ISSN: 2045-8940
Pulmonary arterial hypertension (PAH) is a progressive and debilitating condition. Despite promoting vasodilation, current drugs have a therapeutic window within which they are limited by systemic side effects. Nanomedicine uses nanoparticles to improve drug delivery and/or reduce side effects. We hypothesize that this approach could be used to deliver PAH drugs avoiding the systemic circulation. Here we report the use of iron metal organic framework (MOF) MIL-89 and PEGylated MIL-89 (MIL-89 PEG) as suitable carriers for PAH drugs. We assessed their effects on viability and inflammatory responses in a wide range of lung cells including endothelial cells grown from blood of donors with/without PAH. Both MOFs conformed to the predicted structures with MIL-89 PEG being more stable at room temperature. At concentrations up to 10 or 30 µg/mL, toxicity was only seen in pulmonary artery smooth muscle cells where both MOFs reduced cell viability and CXCL8 release. In endothelial cells from both control donors and PAH patients, both preparations inhibited the release of CXCL8 and endothelin-1 and in macrophages inhibited inducible nitric oxide synthase activity. Finally, MIL-89 was well-tolerated and accumulated in the rat lungs when given in vivo. Thus, the prototypes MIL-89 and MIL-89 PEG with core capacity suitable to accommodate PAH drugs are relatively non-toxic and may have the added advantage of being anti-inflammatory and reducing the release of endothelin-1. These data are consistent with the idea that these materials may not only be useful as drug carriers in PAH but also offer some therapeutic benefit in their own right.
Jin X, Davies RP, 2017, Copper-catalysed aromatic-Finkelstein reactions with amine-based ligand systems, Catalysis Science & Technology, Vol: 7, Pages: 2110-2117, ISSN: 2044-4753
A new efficient and low-cost ligand, diethylenetriamine, has been utilised to promote the iodination of 16 different bromo-substrates via the copper catalysed Finkelstein halogen exchange reaction under mild conditions. In contrast to earlier methods, the use of inert atmosphere conditions was not required to obtain high yields and purity. Studies on the speciation of the catalyst in solution indicate rapid disproportionation of copper(I) in the presence of diethylenetriamine to give copper(0) and a bis-ligated copper(II) complex which is characterised by X-ray diffraction. This copper(II) complex was also shown to be catalytically active in the halogen exchange reaction. In contrast, no significant disproportionation was observed using dimethylethylenediamine as the ligand, and the solid-state structures of a copper(I) dimeric complex and a 2D polymeric network of copper(I) iodide tetramers are reported. The catalytic activity of diethylenetriamine and dimethylethylenediamine with both copper(I) and copper(II) salts are compared, and possible mechanistic implications discussed.
Aragoni MC, Arca M, Coles SJ, et al., 2016, Coordination polymers and polygons using di-pyridyl-thiadiazole spacers and substituted phosphorodithioato Ni II complexes: potential and limitations for inorganic crystal engineering, CrystEngComm, Vol: 18, Pages: 5620-5629, ISSN: 1466-8033
Coordinatively unsaturated P-substituted dithiophosphonato, dithiophosphato, and dithiophosphito complexes {[Ni((MeO)2PS2)2] (1), [Ni((EtO)2PS2)2] (2), [Ni(MeOdtp)2] (3), and [Ni((Ph)2PS2)2] (4)} were reacted with the bis-functional ligands 3,5-di-(4-pyridyl)-1,2,4-thiadiazole (L1) and 3,5-di-(3-pyridyl)-1,2,4-thiadiazole (L2) to give the coordination polymers (1–4·L1)∞, (3·L2)∞, and (4·L2·2C7H8)∞ and the discrete dimers (1–2·L2)2, all characterised by single crystal X-ray diffraction. A comparison of the structures shows that L1 can be exploited for the predictable assembly of undulating chains independent of the nature of the NiII complex, while L2 allows for the existence of different supramolecular constructs ensuing from different ligand conformations deriving from the rotation of the pyridyl rings.
Sung S, Sale D, Braddock DC, et al., 2016, Mechanistic studies on the copper-catalyzed N-arylation of alkylamines promoted by organic soluble ionic bases, ACS Catalysis, Vol: 6, Pages: 3965-3974, ISSN: 2155-5435
Experimental studies on the mechanism of copper-catalyzed amination of aryl halides have been undertaken for the coupling of piperidine with iodobenzene using a Cu(I) catalyst and the organic base tetrabutylphosphonium malonate (TBPM). The use of TBPM led to high reactivity and high conversion rates in the coupling reaction, as well as obviating any mass transfer effects. The often commonly employed O,O-chelating ligand 2-acetylcyclohexanone was surprisingly found to have a negligible effect on the reaction rate, and on the basis of NMR, calorimetric, and kinetic modeling studies, the malonate dianion in TBPM is instead postulated to act as an ancillary ligand in this system. Kinetic profiling using reaction progress kinetic analysis (RPKA) methods show the reaction rate to have a dependence on all of the reaction components in the concentration range studied, with first-order kinetics with respect to [amine], [aryl halide], and [Cu]total. Unexpectedly, negative first-order kinetics in [TBPM] was observed. This negative rate dependence in [TBPM] can be explained by the formation of an off-cycle copper(I) dimalonate species, which is also argued to undergo disproportionation and is thus responsible for catalyst deactivation. The key role of the amine in minimizing catalyst deactivation is also highlighted by the kinetic studies. An examination of the aryl halide activation mechanism using radical probes was undertaken, which is consistent with an oxidative addition pathway. On the basis of these findings, a more detailed mechanistic cycle for the C–N coupling is proposed, including catalyst deactivation pathways.
Mohamed NA, Ahmetaj-Shala B, Duluc L, et al., 2016, A New NO-Releasing Nanoformulation for the Treatment of Pulmonary Arterial Hypertension., Journal of Cardiovascular Translational Research, Vol: 9, Pages: 162-164, ISSN: 1937-5395
Pulmonary arterial hypertension (PAH) is a chronic and progressive disease which continues to carry an unacceptably high mortality and morbidity. The nitric oxide (NO) pathway has been implicated in the pathophysiology and progression of the disease. Its extremely short half-life and systemic effects have hampered the clinical use of NO in PAH. In an attempt to circumvent these major limitations, we have developed a new NO-nanomedicine formulation. The formulation was based on hydrogel-like polymeric composite NO-releasing nanoparticles (NO-RP). The kinetics of NO release from the NO-RP showed a peak at about 120 min followed by a sustained release for over 8 h. The NO-RP did not affect the viability or inflammation responses of endothelial cells. The NO-RP produced concentration-dependent relaxations of pulmonary arteries in mice with PAH induced by hypoxia. In conclusion, NO-RP drugs could considerably enhance the therapeutic potential of NO therapy for PAH.
Grigoropoulos A, Whitehead GFS, Perret N, et al., 2016, Encapsulation of an organometallic cationic catalyst by direct exchange into an anionic MOF, Chemical Science, Vol: 7, Pages: 2037-2050, ISSN: 2041-6539
Metal–Organic Frameworks (MOFs) are porous crystalline materials that have emerged as promising hosts for the heterogenization of homogeneous organometallic catalysts, forming hybrid materials which combine the benefits of both classes of catalysts. Herein, we report the encapsulation of the organometallic cationic Lewis acidic catalyst [CpFe(CO)2(L)]+ ([Fp–L]+, Cp = η5-C5H5, L = weakly bound solvent) inside the pores of the anionic [Et4N]3[In3(BTC)4] MOF (H3BTC = benzenetricarboxylic acid) via a direct one-step cation exchange process. To conclusively validate this methodology, initially [Cp2Co]+ was used as an inert spatial probe to (i) test the stability of the selected host; (ii) monitor the stoichiometry of the cation exchange process and (iii) assess pore dimensions, spatial location of the cationic species and guest-accessible space by single crystal X-ray crystallography. Subsequently, the quasi-isosteric [Fp–L]+ was encapsulated inside the pores via partial cation exchange to form [(Fp–L)0.6(Et4N)2.4][In3(BTC)4]. The latter was rigorously characterized and benchmarked as a heterogeneous catalyst in a simple Diels–Alder reaction, thus verifying the integrity and reactivity of the encapsulated molecular catalyst. These results provide a platform for the development of heterogeneous catalysts with chemically and spatially well-defined catalytic sites by direct exchange of cationic catalysts into anionic MOFs.
Saleem H, Rafique U, Davies RP, 2016, Investigations on post-synthetically modified UiO-66-NH2 for the adsorptive removal of heavy metal ions from aqueous solution, MICROPOROUS AND MESOPOROUS MATERIALS, Vol: 221, Pages: 238-244, ISSN: 1387-1811
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- Citations: 231
Campbell J, Burgal JDS, Szekely G, et al., 2016, Hybrid polymer/MOF membranes for Organic Solvent Nanofiltration (OSN): chemical modification and the quest for perfection, Journal of Membrane Science, Vol: 503, Pages: 166-176, ISSN: 1873-3123
One of the main challenges in the field of Organic Solvent Nanofiltration (OSN) is to improve the selectivity of membranes, allowing the separation of closely related solutes. This objective might be achieved by constructing membranes with uniform porous structures. Hybrid Polymer/Metal Organic Framework (MOF) membranes were prepared by in-situ growth (ISG) of HKUST-1 within the pores of polyimide membranes. To improve the performances of ISG membranes, chemical modification was performed. Aryl carboxylic acid moieties were introduced to polyimide P84 ultrafiltration membranes allowing coordination of the HKUST-1 directly on to the polymer. Chemically modified ISG membranes outperformed non-modified ISG membranes in both solute retentions and permeance. Retentions of polystyrene solute in acetone were used to calculate theoretical pore size distributions for each of the membranes tested. It was found that the chemically modified ISG membrane had he narrowest calculated pore size distribution.
Mohamed NA, Davies R, Lickiss PD, et al., 2016, In Vivo Assessment of Metal Organic Framework (MOFs) for the Future use as Delivery Agents for Drugs to Treat PAH
Pulmonary arterial hypertension (PAH) is a progressive, debilitating and fatal condition with no cure. However small molecule drugs, including sildenafil, selexipag and bosentan, have been developed and are used to treat PAH but do not offer a cure and life expectancy, even on medication, is only between 2-5 years after diagnosis. All PAH drugs are ubiquitous dilators and their therapeutic dose is severely limited by their systemic side-effects [1]. We are working on the hypothesis that current PAH-drugs could be used more effectively at higher local (to the lung) concentrations if delivered selectively using a nanomedicine approach. We suggest that if toxicological limitations of nanomedicines can be overcome their use in PAH to delivery current drugs to the lung could turn this fatal disease to a chronic drug-managedcondition. One nanoparticle that we are interested in is from the Materials of Institute Lavoisier (MIL), the so called MIL-89. MIL-89 is an iron based metal organic framework (MOF). MIL-89 is a good candidate for delivery of drugs because (i) it can be tailored to accommodate different drugs including those with the molecular weights of current PAH-medications (MW; 300-500) [2], (ii) it is biocompatible and biodegradable [3]; (iii) it has a large internal surface area and high drug loading capacity; (iv) it is thermally and mechanically stable; and (v) it promises a long drug release-period with the ability to incorporate different functional groups [2, 4-5]. We have previously shown that MIL-89 at concentrations up to 10µg/ml is non-toxic to human lung cells including those from patients with PAH. In the current study we have investigated the effects of MIL-89 in rats in vivo for markers of toxicity. MIL-89 at 50mg/kg was administered (i.p.) for two weeks at days 0, 1, 3, 7, 10 and 14. At each time point rats were weighed, killed, plasma and tissues collected. MIL-89 had no effect on body weight, lung oedema or on plasma markers of organ failur
Sung S, Braddock DC, Armstrong A, et al., 2015, Synthesis, Characterisation and Reactivity of Copper(I) Amide Complexes and Studies on Their Role in the Modified Ullmann Amination Reaction, CHEMISTRY-A EUROPEAN JOURNAL, Vol: 21, Pages: 7179-7192, ISSN: 0947-6539
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- Citations: 19
Campbell J, Davies RP, Braddock DC, et al., 2015, Improving the permeance of hybrid polymer/metal-organic framework (MOF) membranes for organic solvent nanofiltration (OSN) - development of MOF thin films via interfacial synthesis, JOURNAL OF MATERIALS CHEMISTRY A, Vol: 3, Pages: 9668-9674, ISSN: 2050-7488
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- Citations: 113
Campbell J, Szekely G, Davies RP, et al., 2014, Fabrication of hybrid polymer/metal organic framework membranes: mixed matrix membranes versus in situ growth, Journal of Materials Chemistry A, Vol: 2, Pages: 9260-9271, ISSN: 2050-7488
Hybrid polymer/metal organic framework (MOF) membranes have been prepared using either a mixed matrix membrane (MMM) or in situ growth (ISG) approach and were evaluated for application in organic solvent nanofiltration (OSN). MMMs were produced by dispersing pre-formed particles of the MOF HKUST-1 in polyimide P84 dope solutions. MMMs demonstrated both (i) higher rejections of styrene oligomers and (ii) lower flux decline than the polymeric control membranes. Furthermore, an alternative hybrid membrane fabrication methodology – in situ growth (ISG) of HKUST-1 in integrally skinned asymmetric polymer membrane supports – has been successfully demonstrated. Ultrafiltration support membranes were submerged in HKUST-1 precursor solutions in order to promote the growth of MOF within the porous structure of the polymer membranes. The presence of HKUST-1 in the membranes was proven with X-ray powder diffraction (XRPD). Energy-dispersive X-ray spectroscopy (EDX) was used to reveal the distribution of HKUST-1 throughout the ISG membranes, and was found to be even across the surface and throughout the cross-section. The ISG membranes also had higher solute rejections and lower flux decline than the MMMs.
Bomparola R, Davies RP, Hornaeur S, et al., 2014, Lithium heterocuprates: the influence of the amido group on organoamidocuprate structures, DALTON TRANSACTIONS, Vol: 43, Pages: 14359-14367, ISSN: 1477-9226
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- Citations: 6
Timokhin I, White AJP, Lickiss PD, et al., 2014, Microporous metal-organic frameworks built from rigid tetrahedral tetrakis(4-tetrazolylphenyl)silane connectors, CRYSTENGCOMM, Vol: 16, Pages: 8094-8097, ISSN: 1466-8033
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Davies RP, Patel L, 2013, Chalcogen-Phosphorus (and Heavier Congener) Compounds, Handbook of Chalcogen Chemistry, New Perspectives in Sulfur, Selenium and Tellurium. 2nd Edition. Volume 1, Editors: Devillanova, du Mont, Publisher: The Royal Society of Chemistry, ISBN: 9781849736237
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