A complex of cobalamin with an organic peroxide

Lehene, Maria; Zăgrean-Tuza, Cezara; Hădade, Niculina; Aghion, Andreea; Şeptelean, Raluca; Iancu, Stefania D.; Brânzanic, Adrian M.V.; Silaghi-Dumitrescu, Radu

doi:10.1039/d3nj03307d

New J. Chem.

2023

DOI: 10.1039/d3nj03307d

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A complex of cobalamin with an organic peroxide

Maria Lehene,

Cezara Zăgrean-Tuza,

Niculina Hădade

et al.

Abstract: Aquacobalamin reacts with m-chloroperoxybenzoic acid (MCPBA) to form a Co(III)-peroxo complex, as supported by UV-vis, NMR and resonance Raman spectra complemented by mass spectra and density functional calculations. At high...

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2024

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References 49 publications

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The chlorite adduct of aquacobalamin: contrast with chlorite dismutase

Lehene,

Zagrean-Tuza,

Iancu

et al. 2024

Preprint

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In the reaction of aquacobalamin (aquaCbl) with chlorite, a stable species is detected and assigned as a Co(III)-chlorite complex, Co(III)-OClO−. Its UV-vis spectrum is almost identical to that of aquaCbl, except for some minor differences at ~ 430 nm; cyanide can eliminate and prevent these changes. The 1H-NMR spectra reveal strong influences of chlorite on the B2 and B4 protons of the cobalt-bound dimethyl benzimidazole ligand. Together, the UV-vis and NMR titrations suggest a Kd of 10 mM or higher for chlorite on Cbl. Resonance Raman spectra reveal minor changes in the spectrum of aquaCbl to chlorite – as well as a disappearance of the free chlorite signals, consistent with Cbl-chlorite complex formation. Corroboration for these interpretations is also offered from mass spectrometry and DFT calculations. This Co(III)-OClO− complex would be a stable analogue of the first reaction intermediate in the catalytic cycle of chlorite dismutase, or in the reaction of chlorite with a number of other heme proteins. The differences in reactivity between Co(III) cobalamin and Fe(III) heme towards chlorite are analyzed and rationalized, leading to a reconciliation of experimental and computational data for the latter.

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The chlorite adduct of aquacobalamin: contrast with chlorite dismutase

Lehene,

Zagrean-Tuza,

Iancu

et al. 2024

Preprint

View full text Add to dashboard Cite

show abstract

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A complex of cobalamin with an organic peroxide

Abstract: Aquacobalamin reacts with m-chloroperoxybenzoic acid (MCPBA) to form a Co(III)-peroxo complex, as supported by UV-vis, NMR and resonance Raman spectra complemented by mass spectra and density functional calculations. At high...

Cited by 1 publication

References 49 publications

The chlorite adduct of aquacobalamin: contrast with chlorite dismutase

The chlorite adduct of aquacobalamin: contrast with chlorite dismutase

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