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

Goldberg, Nathaniel and Knight, Anders M. and Zhang, Ruijie and Arnold, Frances H. (2019) Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Cofactors. . (Unpublished) https://resolver.caltech.edu/CaltechAUTHORS:20200227-102506840

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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.

Item Type:

Report or Paper (Discussion Paper)

Related URLs:

URL	URL Type	Description
https://doi.org/10.26434/chemrxiv.10062044.v1	DOI	Discussion Paper

ORCID:

Author	ORCID
Goldberg, Nathaniel	0000-0003-0201-8856
Knight, Anders M.	0000-0001-9665-8197
Zhang, Ruijie	0000-0002-7251-5527
Arnold, Frances H.	0000-0002-4027-364X

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.

Funders:

Funding Agency	Grant Number
NSF	MCB-1513007
NIH Predoctoral Fellowship	T32 GM07616
NIH Predoctoral Fellowship	T32 GM112592
NSF Graduate Research Fellowship	DGE-1144469

DOI:

10.26434/chemrxiv.10062044.v1

Record Number:

CaltechAUTHORS:20200227-102506840

Persistent URL:

https://resolver.caltech.edu/CaltechAUTHORS:20200227-102506840

Usage Policy:

No commercial reproduction, distribution, display or performance rights in this work are provided.

ID Code:

101613

Collection:

CaltechAUTHORS

Deposited By:

Tony Diaz

Deposited On:

27 Feb 2020 19:39

Last Modified:

16 Nov 2021 18:04

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