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Cobaltocene-mediated catalytic monooxygenation using holo and heme domain cytochrome P450 BM3

Udit, Andrew K. and Arnold, Frances H. and Gray, Harry B. (2004) Cobaltocene-mediated catalytic monooxygenation using holo and heme domain cytochrome P450 BM3. Journal of Inorganic Biochemistry, 98 (9). pp. 1547-1550. ISSN 0162-0134. doi:10.1016/j.jinorgbio.2004.06.007. https://resolver.caltech.edu/CaltechAUTHORS:20180821-155119382

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Abstract

The feasibility of replacing NADPH with 1,1′-dicarboxycobaltocene in the catalytic cycle of cytochrome P450 BM3 has been explored. Using the holoprotein, the surrogate mediator was observed to reduce both the FAD and FMN in the reductase domain, as well as the iron in the heme domain. In an electrochemical system, the mediator was able to support lauric acid hydroxylation at a rate of 16.5 nmol product/nmol enzyme/minute. Similar electron transfer and catalysis were observed for the heme domain alone in the presence of the metallocene; the turnover rate in this case was 1.8 nmol product/nmol enzyme/minute. Parallel studies under the same conditions using a previously reported cobalt sepulchrate mediator showed that the two systems give similar results for both the holoenzyme and the heme domain.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.jinorgbio.2004.06.007DOIArticle
ORCID:
AuthorORCID
Arnold, Frances H.0000-0002-4027-364X
Gray, Harry B.0000-0002-7937-7876
Additional Information:© 2004 Elsevier Inc. Received 4 May 2004, Revised 7 June 2004, Accepted 15 June 2004, Available online 5 August 2004. Susan Schofer (Caltech) for assistance with the chemical synthesis; Mike Hill (Occidental College) for helpful discussions; NSF (HBG) and NSERC (Canada) (AKU) for research support.
Funders:
Funding AgencyGrant Number
NSFUNSPECIFIED
Natural Sciences and Engineering Research Council of Canada (NSERC)UNSPECIFIED
Subject Keywords:Cytochrome P450 BM3; Mediator; Electrochemistry; Biocatalysis
Issue or Number:9
DOI:10.1016/j.jinorgbio.2004.06.007
Record Number:CaltechAUTHORS:20180821-155119382
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180821-155119382
Official Citation:Andrew K. Udit, Frances H. Arnold, Harry B. Gray, Cobaltocene-mediated catalytic monooxygenation using holo and heme domain cytochrome P450 BM3, Journal of Inorganic Biochemistry, Volume 98, Issue 9, 2004, Pages 1547-1550, ISSN 0162-0134, https://doi.org/10.1016/j.jinorgbio.2004.06.007. (http://www.sciencedirect.com/science/article/pii/S0162013404001783)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:88996
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:21 Aug 2018 22:57
Last Modified:16 Nov 2021 00:31

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