The development of new approaches to the activation and functionalisation of carbon monoxide and carbon dioxide is a highly topical and significant challenge for chemistry. The use of biomass and coal derived carbon monoxide as a fundamental building block for simple organic molecules is a key objective in energy research, and the latter, coupled with global warming considerations, dictate that new ways to both activate and derivatise carbon dioxide must also be found. The programme of work described in this proposal tackles these problems through experience and excellence in organometallic chemistry and small molecule activation. It is centred around three closely integrated and synergistic strands. The synthetic work in Strand 1 focuses on reductive assembly of carbon monoxide and carbon dioxide on low oxidation state metal centres to build simple organic molecules and rings stoichiometrically. The work in this strand will also be driven by developing a detailed understanding of the mechanisms of these reactions through experiment. A key feature of this proposal is the computational work, which is the subject of Strand 2, in which theory and modelling will be used in an iterative way to predict and inform the experimental synthetic and mechanistic work in Strand 1. Strand 3 will establish the underlying redox properties of these systems using electrochemical techniques, in order to ultimately to generate systems which will catalytically generate organic molecules from carbon monoxide and carbon dioxide. The program of work described in this proposal, which will deliver stoichiometric and catalytic recycling of carbon oxides, is at the frontier of future sustainable chemical technology. It is therefore of high risk, but ultimately extremely high reward.
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