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Understanding Active Site Chemistry of Monoterpene Synthases


EMSL Project ID
51732

Abstract

We propose to use EMSL supercomputing resources to continue gaining a molecular level understanding on the catalytic mechanisms of monoterpene synthases (MTSs). Specifically, we will perform an extensive set of atomistic simulations to elucidate how steric and electrostatic confinement affect the conformational space of highly reactive carbocation intermediates in MTSs. Based on the previous studies supported by EMSL supercomputing resources, we will continue exploring the conformational space of reaction intermediates and find key amino acids that influence enzyme specificity and selectivity by using molecular dynamics (MD) simulations and hybrid QM/MM methods. Our computational results will be iteratively compared with the corresponding experimental results provided by our collaborator at Washington State University (WSU) to validate expected reaction paths and a role of key amino acids observed from computational approaches. This research is a key component of DOE Basic Energy Science Physical Bioscience program at PNNL.

Project Details

Start Date
2020-10-20
End Date
2021-09-30
Status
Closed

Team

Principal Investigator

Simone Raugei
Institution
Pacific Northwest National Laboratory

Team Members

Hoshin Kim
Institution
Pacific Northwest National Laboratory

Bojana Ginovska
Institution
Pacific Northwest National Laboratory

Related Publications

Hoshin Kim, Narayanan Srividya, Iris Lange, Eden W. Huchala, Bojana Ginovska, B. Markus Lange, Simone Raugei. 2022. "Determinants of Selectivity for the Formation of Monocyclic and Bicyclic Products in Monoterpene Synthases." ACS Catalysis 12 (12):7453-7469. https://pubs.acs.org/doi/full/10.1021/acscatal.2c01836