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Published November 5, 2019 | Submitted + Supplemental Material
Discussion Paper Open

Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Cofactors

Goldberg, Nathaniel ORCID icon
Knight, Anders M. ORCID icon
Zhang, Ruijie ORCID icon
Arnold, Frances H. ORCID icon
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Abstract

Transition-metal catalysis is a powerful tool for the construction of chemical bonds. Here we show that a non-heme iron enzyme can catalyze olefin aziridination and nitrene C–H insertion, and that these activities can be improved by directed evolution. The non-heme iron center allows for facile modification of the primary coordination sphere by addition of metal-coordinating molecules, enabling control over enzyme activity and selectivity using small molecules.

Additional Information

LICENCE: CC BY-NC-ND 4.0. Submission date: 30.10.2019; First online date Posted date: 05.11.2019. This work was supported by the National Science Foundation (NSF) Division of Molecular and Cellular Biosciences (grant MCB-1513007). N. W. G., A. M. K., and R. K. Z. acknowledge support from the NIH training grants NIH T32 GM07616 (N. W. G.) and NIH T32 GM112592 (A. M. K., R. K. Z.) and NSF Graduate Research Fellowship DGE-1144469 (A. M. K, R. K. Z.). We thank Sabine Brinkmann-Chen for critical reading of the manuscript and Noah P. Dunham, S. B. Jennifer Kan, and Benjamin J. Levin for helpful discussions. We thank Professor Hans Renata and Professor Harry Gray for generously sharing plasmids. A provisional patent has been filed through the California Institute of Technology based on the results presented here.

Attached Files

Submitted - Nitrene_Transfer_Catalyzed_by_a_Non-Heme_Iron_Enzyme_and_Enhanced_by_Non-Native_Small-Molecule_Cofactors_v1.pdf

Supplemental Material - EFE_SI_20191028.pdf

Files

Nitrene_Transfer_Catalyzed_by_a_Non-Heme_Iron_Enzyme_and_Enhanced_by_Non-Native_Small-Molecule_Cofactors_v1.pdf

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