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  • Switchable Molecules: A Radical Approach

Switchable Molecules: A Radical Approach

The majority of the ligands used in metal complexes are not 'redox-active', that is, any redox processes in such materials are dominated by the metal centre. A more interesting route involves so called 'redox-active' ligands which undergo redox processes before the metal centre. When used in tandem with a suitable choice of metal they have the potential to facilitate multielectron transformations and are obvious candidates to replace the catalytic processes commonly found in expensive and scarce noble metals like platinum or irridum. This is typified by aerobic alcohol oxidation catalysts such as those reported by Stahl et al. which are chemoselective and high yielding. Metal complexes containing 'redox active' ligands have also been utilised to great effect in molecular magnetism, biomimetic studies of redox-active metalloenzymes, quantum computing, and molecular spintronics. 

Our initial foray into radical inorganic chemistry involved a nitroxide based 'redox-active' ligand and was a study of the interplay between radical–metal exchange and spin-crossover properties of a small series of iron and cobalt metal radical complexes. This revealed small redox active molecules which could undergo significant physical and electronic changes offering a unique switchable system. Such advanced materials will be explored to probe their fundamental and applied properties.

molecular-model-one-third-full-image

Molecular structure of the metal radical cation

Redox-processes-in-the-metal-radical-cation

Redox processes in the metal radical cation

Project timeframe

The project runs from 2014 to 2018.

Project aims

We are currently investigating the fundamental properties of a host of metal-radical complexes and their potential use in molecular electronics, molecular magnetism, biosensors and catalysis.

Project findings and impact

A combination of iron and a tridentate nitroxide radical chelating ligand resulted in a unique switchable system where a dicationic species [FeII(L•)2]2+ undergoes a reductively induced oxidationto form a monocationic species [FeIII(L-)2]+ and vice versa. When the central metal is changed from iron to cobalt or manganese we generate multifunctional materials capable of solvate-dependent spin-crossover and magnetic exchange, multiple redox processes and single-molecule magnet (SMM) properties. Very small perturbations to these systems can dramatically affect their electronic properties. This switchable effect could be utilised in a variety of applications across the chemical and biological sciences.

Research team

Simon Easton

Blaise Geoghegan

Jack Bailey

Robert Preston

Jess Lewis

Ian A Gass

Output

Solvate-Dependent Spin Crossover and Exchange in Cobalt(II) Oxazolidine Nitroxide Chelates, I. A. Gass, S. Tewary, G. Rajaraman, M. Asadi, D. W. Lupton, B. Moubaraki, G. Chastanet, J.-F. Létard, K. S. Murray, Inorg. Chem., 2014, 53, 5055.

Manganese(II) Oxazolidine Nitroxide Chelates: Structure, Magnetism, and Redox Properties, I. A. Gass, M, Asadi, D. W. Lupton, B. Moubaraki, A. M. Bond, S.-X. Guo, K. S. Murray, Aus. J. Chem., 2014, 67, 1618.

Ferromagnetic exchange, Spin-crossover, Reductively Induced Oxidation and Field Induced Slow Magnetic Relaxation in Monomeric Cobalt Nitroxides. I. A. Gass, S. Tewary, A. Nefady N. F. Chilton, C. J. Gartshore, M. Asadi, D. W. Lupton, B. Moubaraki, A. M. Bond, J. F. Boas, S.-X. Guo, G. Rajaraman, K. S. Murray, Inorg Chem., 2013, 52, 7557.

Theoretical Perspectives on Redox “Non-innocent” Oxazolidine-N-oxide Iron Nitroxide Complexes, S. Tewary, I. A. Gass, K. S. Murray, G. Rajaraman, , Eur. J. Inorg. Chem., 2013, 5-6, 1024.

Anion Dependent Redox Changes in Iron bis-terdentate Nitroxide {NNO} Chelates I. A. Gass, C. J. Gartshore, D. W. Lupton, B. Moubaraki, A. Nafady, A. M. Bond, J. F. Boas, J. D. Cashion, C. Milsmann, K. Wieghardt, K. S. Murray, Inorg. Chem., 2011, 50, 3052.

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