Electrochemical generation of a high-valent state of cytochrome P450

Journal of Inorganic Biochemistry
Andrew K UditHarry B Gray

Abstract

Cyclic voltammetry performed at rapid scan rates on cytochrome P450 from Pseudomonas putida (P450CAM) in didodecyldimethylammonium bromide (DDAB) films on graphite electrodes revealed a couple (E) at 830mV (vs Ag/AgCl). E was not significantly observed at scan rates less than 30V/s at room temperature, suggesting that the oxidized species is unstable. The lifetime of E could be prolonged at 4 degrees C, which allowed reversible access to E at scan rates as low as 1V/s. E was found to be sensitive to imidazole in solution and to variations in pH, suggesting that the redox reaction is occurring at the metal center (i.e., Fe(IV/III)). Electrolysis reactions with different P450 substrates revealed that the electrochemically generated high-valent species is able to convert thioanisole to methyl phenyl sulfoxide.

References

Feb 24, 2001·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·T EgawaY Ishimura
Oct 9, 2002·Nature Biotechnology·Anton GliederFrances H Arnold
Oct 2, 2003·European Journal of Biochemistry·Barry D FlemingH Allen O Hill
Oct 9, 2003·Journal of the American Chemical Society·Alexander R DunnHarry B Gray
Mar 3, 2004·Molecular Interventions·F Peter Guengerich
Apr 24, 2004·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Radu Silaghi-Dumitrescu
Jul 15, 2004·Journal of the American Chemical Society·Emek BlairPatrick J Farmer
Aug 19, 2004·Journal of the American Chemical Society·Andrew K UditHarry B Gray
Aug 11, 2005·Journal of the American Chemical Society·Andrew K UditHarry B Gray

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Citations

Jan 23, 2016·Environmental Science and Pollution Research International·Shan-Wei LiGuo-Ping Sheng
Jun 19, 2010·Biochimica Et Biophysica Acta·Christiane Jung
May 2, 2018·Chemical Communications : Chem Comm·Wuyuan Zhang, Frank Hollmann

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