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Taming of a Poison: Biosynthesis of the NiFe-Hydrogenase Cyanide Ligands

Science  14 Feb 2003:
Vol. 299, Issue 5609, pp. 1067-1070
DOI: 10.1126/science.1080972

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Abstract

NiFe-hydrogenases have an Ni-Fe site in which the iron has one CO and two CN groups as ligands. Synthesis of the CN ligands requires the activity of two hydrogenase maturation proteins: HypF and HypE. HypF is a carbamoyltransferase that transfers the carbamoyl moiety of carbamoyladenylate to the COOH-terminal cysteine of HypE and thus forms an enzyme-thiocarbamate. HypE dehydrates theS-carbamoyl moiety in an adenosine triphosphate–dependent process to yield the enzyme thiocyanate. Chemical model reactions corroborate the feasibility of this unprecedented biosynthetic route and show that thiocyanates can donate CN to iron. This finding underscores a striking parallel between biochemistry and organometallic chemistry in the formation of an iron-cyano complex.

  • * To whom correspondence should be addressed. E-mail: august.boeck{at}lrz.uni-muenchen.de

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