We are interested in making complexes that challenge our preconceived ideas about structure and bonding in early transition metal, and lanthanide and actinide chemistry. This involves the design of ligands to support complexes in unusual formal oxidation states or structural types, and the synthesis of new compounds that have the potential to engage in bonding or redox reactivities that would not be possible in more traditional systems.

We are particularly interested in the activation and functionalisation of hydrocarbon C-H bonds. With N-heterocyclic carbene ligands we are making organometallic f-block complexes that can make new carbon-heteroelement and nitrogen-heteroelement bonds, and high oxidation state late metal complexes that are catalysts for C-H bond halogenation. With rigid Pacman-shaped ligands in collaboration with Dr Love we are studying C-H bond activation by uranium and uranyl complexes. We also routinely test the reactivity of new complexes towards the activation of important small molecules including carbon monoxide and carbon dioxide, dinitrogen, hydrogen, and alkenes and alkanes. Many of the complexes we study also display reactivity as catalysts for organic transformations, such as the conversion of carbon dioxide and other renewable monomers into biodegradable polymers.

We are also involved in both local and international collaborations with other synthetic chemists in the study of some of the reaction chemistry, and with computational chemists to help understand the bonding in the more unusual systems.

SELECTED RECENT PUBLICATIONS

1. Small Molecule Activation by Uranium Tris(aryloxides): Experimental and Computational Studies of Binding of N₂, Coupling of CO and Deoxygenation Insertion of CO₂ under Ambient Conditions S. M. Mansell, N. Kaltsoyannis, P. L. Arnold, J. Am. Chem. Soc., 2011, in press.
See also: Carbon monoxide coupling and functionalisation at a simple uranium coordination complex P. L. Arnold et al, Chem. Sci., 2011, 2, 77-79.
2. Single-electron uranyl reduction by a rare-earth cation P. L. Arnold, E. Hollis, F. J. White, N. Magnani, R. Caciuffo, J. B. Love, Angew. Chem.-Int. Edit., 2011, 50, 887-890.
3. Uranyl oxo activation and functionalisation by metal cation coordination P. L. Arnold, A.-F. Pecharman, E. H. Hollis, A. Yahia, L. Maron, S. Parsons, J. B. Love, Nature Chem., 2010, 2, 1056-1061.
4. Addition - elimination reactions across the M-C bond of metal N-heterocyclic carbenes Z. R. Turner, R. Bellabarba, R. P. Tooze, P. L. Arnold, J. Am. Chem. Soc. 2010, 132, 4050.
5. Reduction and selective oxo-group silylation of the uranyl dication P. L. Arnold, D. Patel, C. Wilson, J. B. Love, Nature 2008, 451, 315. Featured articles appeared: on Nature News; on the BBC; on the Daily Telegraph; on the New Scientist.

Reviews

1. Uranium-mediated activation of small molecules Highlight article, Polly L. Arnold, Chem. Commun, 2011, in press.
2. F-block N-heterocyclic carbene complexes P. L. Arnold, I. J. Casely Chem. Rev. 2009, 109, 3599.

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