Research in the Hyster group focuses on developing new biocatalytic methods to address long-standing reactivity and selectivity challenges in organic synthesis. To this end, we are developing photoenzymatic strategies for generating organic free radicals within protein active sites. Using protein engineering and directed evolution, we can precisely control the reactivity of radical intermediates. This feature enables enzymes to address challenges in the field of organic free-radical chemistry. We are also inventing new biocompatible photoredox reactions, enabling cascade reactions involving small molecule and enzymatic catalysts. These new tools can be applied to challenges encountered by the agrochemical and pharmaceutical industries.
P. J. Clayman, T. K. Hyster “Photoenzymatic Generation of Unstabilized Alkyl Radicals: An Asymmetric Reductive Cyclization” J. Am. Chem. Soc. 2020, 142, 15673-15677.
J. S. DeHovitz, Y. Y. Loh, J. A. Kautzky, K. Nagao, A. J. Meichan, M. Yamauchi, D. W. C. MacMillan, T. K. Hyster, “Inducing Dynamic Stereochemistry for Asymmetric Synthesis” Science 2020, 369, 1113-1118.
Y. Nakano, M. J. Black, A. J. Meichan, B. A. Sandoval, M. M. Chung, K. F. Biegasiewicz, T. Zhu, T. K. Hyster “Synergistic Photoenzymatic Hydrogenation of Heteroaromatic Olefins by ‘Ene’-Reductases.” Angew. Chem. Int. Ed. 2020, 59, 10484-10488.
M. J. Black, A. J. Meichan, K. F. Biegasiewicz, B. Kudisch, D. G. Oblinsky, G. D. Scholes, T. K. Hyster* “Asymmetric Radical Cyclization Enabled by Electron Transfer from Flavin in an ‘Ene’-Reductase” Nat. Chem. 2020, 12, 71-75.
K. F. Biegasiewicz, S. J. Cooper, X. Gao, D. G. Oblinsky, J. H. Kim, S. E. Garfinkle, L. A. Joyce, B. A. Sandoval, G. D. Scholes, T. K. Hyster* “Photoexcitation of a Flavoenzyme Enables a Stereocontrolled Radical Cyclization” Science 2019, 364, 1166-1169.