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PhotoArM - Directed Evolution of Photoredox Powered Artificial Metalloenzymes for Stereodivergent Catalysis

Research Project
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01.04.2019
 - 31.03.2021

Photoredox catalysis has recently been established as a powerful method of achieving unconventional chemical reactivity via open-shell reaction intermediates. In combination with the high reactivity of transition metal catalysis, metallaphotoredox catalysis has allowed the coupling of non-traditional partners under mild conditions. 1 However, achieving these reactions selectively remains an ongoing challenge. 2 Concomitantly, efforts to combine the control offered by enzymes with the expanded reaction repertoire of abiotic cofactors have yielded many examples of artificial metalloenzymes capable of carrying out highly selective unnatural reactions. 3 Unifying the unconventional reactivity of metallaphotoredox catalysis with the unparalleled levels of control offered by enzymes would give a new class of artificial metallaphotoredoxenzymes (PhotoArMs) Herein we investigate the development of novel PhotoArMs based on the biotin-streptavidin technology powered by an external photocatalyst to carry out enantioselective coupling reactions. 1) J. Twilton, C. C. Le, P. Zhang, M. H. Shaw, R. W. Evans and D. W. C. MacMillan, Nat. Rev. Chem. 2017 , 1 , 0052 2) M. Silvi and P. Melchiorre, Nature 2018 , 554 , 41 3) F. Schwizer, Y. Okamoto, T. Heinisch, Y. Gu, M.M. Pellizzoni, V. Lebrun, R. Reuter, V. Köhler, J.C. Lewis and T.R. Ward, Chem. Rev. 2018 , 118 , 142

Funding

PhotoArM - Directed Evolution of Photoredox Powered Artificial Metalloenzymes for Stereodivergent Catalysis

Horizon 2020 Marie Sklodowska-Curie (GrantsTool), 04.2019-03.2021 (24)
PI : Ward, Thomas R..
CI : Davis, Holly Jane.

Members (2)

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Thomas R. Ward

Principal Investigator
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Holly Jane Davis

Co-Investigator