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Nanosecond photoreduction of inducible nitric oxide synthase by a Ru-diimine electron tunneling wire bound distant from the active site

Whited, Charlotte A. and Belliston-Bittner, Wendy and Dunn, Alexander R. and Winkler, Jay R. and Gray, Harry B. (2009) Nanosecond photoreduction of inducible nitric oxide synthase by a Ru-diimine electron tunneling wire bound distant from the active site. Journal of Inorganic Biochemistry, 103 (6). pp. 906-911. ISSN 0162-0134. PMCID PMC2700734. doi:10.1016/j.jinorgbio.2009.04.001. https://resolver.caltech.edu/CaltechAUTHORS:20090904-135737718

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Abstract

A Ru-diimine wire, [(4,4′,5,5′-tetramethylbipyridine)_2Ru(F_9bp)]^(2+) (tmRu-F_9bp, where F_9bp is 4-methyl-4′-methylperfluorobiphenylbipyridine), binds tightly to the oxidase domain of inducible nitric oxide synthase (iNOSoxy). The binding of tmRu-F_9bp is independent of tetrahydrobiopterin, arginine, and imidazole, indicating that the wire resides on the surface of the enzyme, distant from the active-site heme. Photoreduction of an imidazole-bound active-site heme iron in the enzyme-wire conjugate (k_(ET) = 2(1) × 10^7 s^(−1)) is fully seven orders of magnitude faster than the in vivo process.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.jinorgbio.2009.04.001DOIArticle
http://www.sciencedirect.com/science/article/pii/S0162013409000695?via%3DihubPublisherArticle
https://www.ncbi.nlm.nih.gov/pmc/articles/PMC2700734PubMed CentralArticle
ORCID:
AuthorORCID
Dunn, Alexander R.0000-0001-6096-4600
Winkler, Jay R.0000-0002-4453-9716
Gray, Harry B.0000-0002-7937-7876
Additional Information:© 2009 Elsevier. Received 3 December 2008; revised 1 April 2009; accepted 2 April 2009. Available online 17 April 2009. We thank Michael Marletta for the generous gift of protein reagents and for assistance with the iNOS purification protocol. This work was supported by NIH (DK19038 (H.B.G); GM070868 (H.B.G); GM068461 (J.R.W)), by the Fannie and John Hertz Foundation (A.R.D), the Ellison Medical Foundation (Senior Scholar Award in Aging to H.B.G), a NSF graduate research fellowship (C.A.W), and the Arnold and Mabel Beckman Foundation. Supplementary data associated with this article can be found, in the online version, at doi:10.1016/j.jinorgbio.2009.04.001.
Funders:
Funding AgencyGrant Number
NIHDK19038
NIHGM070868
NIHGM068461
Fannie and John Hertz FoundationUNSPECIFIED
Ellison Medical FoundationUNSPECIFIED
NSFUNSPECIFIED
Arnold and Mabel Beckman FoundationUNSPECIFIED
Subject Keywords:Nitric oxide synthase; Electron transfer; Tunneling wire; Ru sensitizer
Issue or Number:6
PubMed Central ID:PMC2700734
DOI:10.1016/j.jinorgbio.2009.04.001
Record Number:CaltechAUTHORS:20090904-135737718
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20090904-135737718
Official Citation:Charlotte A. Whited, Wendy Belliston-Bittner, Alexander R. Dunn, Jay R. Winkler, Harry B. Gray, Nanosecond photoreduction of inducible nitric oxide synthase by a Ru-diimine electron tunneling wire bound distant from the active site, Journal of Inorganic Biochemistry, Volume 103, Issue 6, June 2009, Pages 906-911, ISSN 0162-0134, DOI: 10.1016/j.jinorgbio.2009.04.001. (http://www.sciencedirect.com/science/article/B6TGG-4W38RBW-1/2/1688a880c45c78813a0a14cc4f4bcfb1)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:15628
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:23 Sep 2009 19:06
Last Modified:08 Nov 2021 23:20

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