Published December 18, 2019
| Version Accepted Version + Submitted + Supplemental Material
Journal Article
Open
Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Ligands
Abstract
Transition-metal catalysis is a powerful tool for the construction of chemical bonds. Here we show that Pseudomonas savastanoi ethylene-forming enzyme, 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
© 2019 American Chemical Society. Received: October 28, 2019; Published: December 2, 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 U.S. National Institutes of Health (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. Author Contributions: N.W.G. and A.M.K. contributed equally. The authors declare the following competing financial interest(s): A provisional patent, on which N.W.G., A.M.K., and R.K.Z. are inventors, has been filed through the California Institute of Technology based on the results presented here.Attached Files
Accepted Version - jacs.9b11608_accepted.pdf
Accepted Version - nihms-1062404.pdf
Submitted - EFE_Manuscript_20191028.pdf
Supplemental Material - ja9b11608_si_001.pdf
Supplemental Material - ja9b11608_si_002.xlsx
Files
EFE_Manuscript_20191028.pdf
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Additional details
Additional titles
- Alternative title
- Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Cofactors
Identifiers
- PMCID
- PMC6924163
- Eprint ID
- 100023
- DOI
- 10.1021/jacs.9b11608
- Resolver ID
- CaltechAUTHORS:20191125-092520827
Related works
Funding
- NSF
- MCB-1513007
- NIH Predoctoral Fellowship
- T32 GM07616
- NIH Predoctoral Fellowship
- T32 GM112592
- NSF Graduate Research Fellowship
- DGE-1144469
Dates
- Created
-
2019-11-25Created from EPrint's datestamp field
- Updated
-
2022-02-10Created from EPrint's last_modified field