The Forgan group is broadly interested in self-assembly, with current focus on metal-organic frameworks (MOFs). MOFs are self-assembled constructs wherein metal or metal cluster 'joints' link organic 'struts' to form highly interconnected hollow networks which often display permanent porosity. The ability to trap and store small molecules within MOFs leads to a number of potential applications.
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Enhanced Reactivity in Porous Materials
Metal-organic frameworks contain arrays of ordered nanoscale pores which are often accessible to outside reagents by diffusion throughout the nanoporous network. Confining reagents within these 'molecular flasks' can dramatically alter their reactivity and regioselectivity. The Forgan Group are exploiting this enhanced reactivity phenomenon to generate heterogeneous biomimetic catalysts - artificial enzymes - through extensive pore functionalisation and templated-directed synthesis. These studies (EPSRC grant EP/L004461/1) are underpinned by the Forgan Group's continuous investigations into the fundamentals of molecular recognition within MOFs themselves.
See: “Structure-Directing Factors when Introducing Hydrogen Bond Functionality to Metal-Organic Frameworks” R. S. Forgan, R. J. Marshall, M. Struckmann, A. B. Bleine, D. –L. Long, M. C. Bernini, D. Fairen-Jimenez, CrystEngComm 2015, 17, 299–306.
Drug Delivery from Functionalised Porous NanoMOFs
MOFs are being increasingly utilised to store and deliver molecular cargos to treat disease. The Forgan Group has developed a simple but effective methodology to produce bespoke, highly functionalised MOF nanoparticles to be used as targeted drug delivery vectors. In concert with our continuing interest in the interactions between MOF scaffolds and substrates, we aim to produce theranostic nanomaterials targeted at imaging and remedying specific ailments (ERC Starting Grant 677289).
See: “The Surface Chemistry of Metal-Organic Frameworks” C. V. McGuire and R. S. Forgan, Chem. Commun. 2015, 51, 5199–5217.
Crystallisation and Mechanical Properties of Zr MOFs
The Forgan group has conceived novel synthetic methodologies to enhance the crystallinity of Zr and Hf MOFs, allowing access to single crystals of otherwise unavailable MOFs. These breakthroughs have facilitated comprehensive studies of the MOFs under high pressure, elucidating mechanical properties, and led to the development of new postsynthetic modification protocols with applications in permanent sequestration of toxic gases.
See: “Amino Acids as Highly Efficient Modulators for Single Crystals of Zirconium and Hafnium Metal-Organic Frameworks” R. J. Marshall, C. L. Hobday, C. F. Murphie, S. L. Griffin, C. A. Morrison, S. A. Moggach and R. S. Forgan, J. Mater. Chem. A 2016, 4, 6955–6963.
See: “Geometric Frustration in UiO Frameworks: A Computational and Experimental Approach Linking Disorder, High-Pressure Behaviour and Mechanical Properties” C. L. Hobday, R. J. Marshall, C. F. Murphie, J. Sotelo, T. Richards, D. Allan, T. Düren, F. –X. Coudert, R. S. Forgan, C. A. Morrison, S. A. Moggach and T. D. Bennett, Angew. Chem. Int. Ed. 2016, 55, 2401–2405.
See: “Single-Crystal to Single-Crystal Mechanical Contraction of Metal-Organic Frameworks through Stereoselective Post-Synthetic Bromination” R. J. Marshall, S. L. Griffin, C. Wilson and R. S. Forgan, J. Am. Chem. Soc. 2015, 137, 9527–9530.