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Research Article

Insights into Hydrocarbon Formation by Nitrogenase Cofactor Homologs

Chi Chung Lee, Yilin Hu, Markus W. Ribbe
Douglas G. Capone, Editor
Chi Chung Lee
aDepartment of Molecular Biology and Biochemistry, University of California, Irvine, Irvine, California, USA
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Yilin Hu
aDepartment of Molecular Biology and Biochemistry, University of California, Irvine, Irvine, California, USA
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Markus W. Ribbe
aDepartment of Molecular Biology and Biochemistry, University of California, Irvine, Irvine, California, USA
bDepartment of Chemistry, University of California, Irvine, Irvine, California, USA
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Douglas G. Capone
University of Southern California
Roles: Editor
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DOI: 10.1128/mBio.00307-15
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ABSTRACT

The L-cluster is an all-iron homolog of nitrogenase cofactors. Driven by europium(II) diethylenetriaminepentaacetate [Eu(II)-DTPA], the isolated L-cluster is capable of ATP-independent reduction of CO and CN− to C1 to C4 and C1 to C6 hydrocarbons, respectively. Compared to its cofactor homologs, the L-cluster generates considerably more CH4 from the reduction of CO and CN−, which could be explained by the presence of a “free” Fe atom that is “unmasked” by homocitrate as an additional site for methanation. Moreover, the elevated CH4 formation is accompanied by a decrease in the amount of longer hydrocarbons and/or the lengths of the hydrocarbon products, illustrating a competition between CH4 formation/release and C−C coupling/chain extension. These observations suggest the possibility of designing simpler synthetic clusters for hydrocarbon formation while establishing the L-cluster as a platform for mechanistic investigations of CO and CN− reduction without complications originating from the heterometal and homocitrate components.

IMPORTANCE Nitrogenase is a metalloenzyme that is highly complex in structure and uniquely versatile in function. It catalyzes two reactions that parallel two important industrial processes: the reduction of nitrogen to ammonia, which parallels the Haber-Bosch process in ammonia production, and the reduction of carbon monoxide to hydrocarbons, which parallels the Fischer-Tropsch process in fuel production. Thus, the significance of nitrogenase can be appreciated from the perspective of the useful products it generates: (i) ammonia, the “fixed” nitrogen that is essential for the existence of the entire human population; and (ii) hydrocarbons, the “recycled” carbon fuel that could be used to directly address the worldwide energy shortage. This article provides initial insights into the catalytic characteristics of various nitrogenase cofactors in hydrocarbon formation. The reported assay system provides a useful tool for mechanistic investigations of this reaction while suggesting the possibility of designing bioinspired catalysts based on nitrogenase cofactors.

FOOTNOTES

    • Received 23 February 2015
    • Accepted 25 March 2015
    • Published 14 April 2015
  • Copyright © 2015 Lee et al.

This is an open-access article distributed under the terms of the Creative Commons Attribution-Noncommercial-ShareAlike 3.0 Unported license, which permits unrestricted noncommercial use, distribution, and reproduction in any medium, provided the original author and source are credited.

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Insights into Hydrocarbon Formation by Nitrogenase Cofactor Homologs
Chi Chung Lee, Yilin Hu, Markus W. Ribbe
mBio Apr 2015, 6 (2) e00307-15; DOI: 10.1128/mBio.00307-15

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Insights into Hydrocarbon Formation by Nitrogenase Cofactor Homologs
Chi Chung Lee, Yilin Hu, Markus W. Ribbe
mBio Apr 2015, 6 (2) e00307-15; DOI: 10.1128/mBio.00307-15
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