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Multi-scale investigation of the nitrogen fixation mechanism of Mo-dependent nitrogenase


EMSL Project ID
48288

Abstract

We propose to use EMSL NMR and supercomputing resources to gain a molecular level understanding of how substrate binding, electron, and proton delivery is controlled by the nitrogenase metalloenzyme to synthesize ammonia (NH3) from dinitrogen (N2). This research is a key component of the DOE Basic Energy Sciences Physical Biosciences proposal at PNNL, aimed at characterizing key biochemical and biophysical features of enzymatic processes and translate catalytic principles from enzymes' activity to synthetic robust catalytic platforms. We propose to use EMSL NMR and multi-scale computational studies to (1) test reaction pathways, calculate structures and energy profiles for N2 reduction intermediates, and (2) characterize large-amplitude protein fluctuations gating the electron transport steps. Characterization of structural, dynamic and thermodynamic aspects of ammonia synthesis by nitrogenase is expected to yield insights that will inform the development of functional biomimetic catalysts, which are more efficient and environmentally friendly than industrial processes currently in use.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2014-10-01
End Date
2016-09-30
Status
Closed

Team

Principal Investigator

Simone Raugei
Institution
Pacific Northwest National Laboratory

Team Members

Noopur Sharma
Institution
Environmental Molecular Sciences Laboratory

Lewis EV Johnson
Institution
Pacific Northwest National Laboratory

Brian Hoffman
Institution
Northwestern University

Lance Seefeldt
Institution
Utah State University

James Evans
Institution
Environmental Molecular Sciences Laboratory

Bojana Ginovska
Institution
Pacific Northwest National Laboratory

Wendy Shaw
Institution
Pacific Northwest National Laboratory

Dayle Smith
Institution
Intel Corporation