Concentration-dependent front velocity of the autocatalytic hydrogenase reaction

Gabriella Bodó, Rui M M Branca, A. Tóth, D. Horváth, Csaba Bagyinka

Research output: Contribution to journalArticle

9 Citations (Scopus)

Abstract

HynSL hydrogenase from Thiocapsa roseopersicina was applied to catalyze the oxidation of molecular hydrogen in a new, improved, thin-layer reaction chamber. Investigation of the nature of this catalysis via the development of reduced benzyl viologen showed clearly the typical characteristics of an autocatalytic reaction: propagation of a reaction front originating from a single point, with a constant velocity of front propagation. The dependence of the reaction velocity on enzyme concentration was a power function with a positive enzyme concentration threshold, with an exponent of 0.4 ± 0.05. This indicates that the autocatalyst is an enzyme form. The front velocity decreased on increase of the electron acceptor concentration, as a sign that the autocatalyst interacts directly with the final electron acceptor. Overall, it may be concluded that the autocatalyst is an enzyme form in which [FeS] distal is reduced. Model calculations corroborate this. Because the reduction of all [FeS] clusters would be possible in a nonautocatalytic reaction, we hypothesize a small conformational change in the enzyme, catalyzed by the autocatalyst, which removes a block in the electron flow in either [NiFe] → [FeS]proximal or the [FeS]proximal → [FeS]distal reaction step, or removes a block of the penetration of gaseous hydrogen from the surface to the [NiFe] cluster.

Original languageEnglish
Pages (from-to)4976-4983
Number of pages8
JournalBiophysical Journal
Volume96
Issue number12
DOIs
Publication statusPublished - 2009

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Hydrogenase
Enzymes
Electrons
Thiocapsa roseopersicina
Hydrogen
Benzyl Viologen
Catalysis

ASJC Scopus subject areas

  • Biophysics

Cite this

Concentration-dependent front velocity of the autocatalytic hydrogenase reaction. / Bodó, Gabriella; Branca, Rui M M; Tóth, A.; Horváth, D.; Bagyinka, Csaba.

In: Biophysical Journal, Vol. 96, No. 12, 2009, p. 4976-4983.

Research output: Contribution to journalArticle

Bodó, Gabriella ; Branca, Rui M M ; Tóth, A. ; Horváth, D. ; Bagyinka, Csaba. / Concentration-dependent front velocity of the autocatalytic hydrogenase reaction. In: Biophysical Journal. 2009 ; Vol. 96, No. 12. pp. 4976-4983.
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