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

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

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

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Additional details

Identifiers

Eprint ID
101613
Resolver ID
CaltechAUTHORS:20200227-102506840

Funding

NSF
MCB-1513007
NIH Predoctoral Fellowship
T32 GM07616
NIH Predoctoral Fellowship
T32 GM112592
NSF Graduate Research Fellowship
DGE-1144469

Dates

Created
2020-02-27
Created from EPrint's datestamp field
Updated
2021-11-16
Created from EPrint's last_modified field

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