The direct transformation of a C-H bond to a C-X bond (X = O, N, C) is pivotal to improving the environmental sustainability of organic chemistry. The development of transition metal catalysts for these reactions has led to outstanding achievements in selective transformations and their resulting applications in synthesis. However, many of these reactions still rely on the heavier and more expensive transition metals (Rh, Ir, Pt, Pd). Ideally, it would be beneficial to replace these metals with more abundant metal catalysts such as Fe or Cu, and to create catalysts that are easily recoverable from reactions mixtures i.e. filtration of solid supported catalysts. First row transition metals are used by nature to carry out many biologically relevant transformation such as oxidations. Recent work has shown that Fe-heme enzymes can be repurposed for non-natural reactions using nitrenes and carbene, which are isoelectronic with the natural Fe-oxo intermediates,[1] whilst artificial metalloenzymes (ArMs) have also been developed for catalysis with abundant metals such as Cu.[2]
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We are interested in increasing the activity of catalysts based on the late-transition metals by incorporating them into artificial enzymes, and investigating catalysts based on more abundant metals that may replace these in the future.
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1. Hammer, S. C., Knight, A. M., Arnold, F. H. Curr. Opin. Green Sus. Chem. 2017, 7, 23.
2. Mann, S. I, Heinisch, T., Ward, T. R., Borovik, A. S. J. Am. Chem. Soc. 2017, ASAP: 10.1021/jacs.7b10452