Ether cross-link formation in the R2-like ligand-binding oxidase

Griese, Julia J. (author): Uppsala universitet,Stockholms universitet,Institutionen för biokemi och biofysik,Uppsala University, Sweden,Strukturbiologi,Stockholm Univ, Dept Biochem & Biophys, S-10691 Stockholm, Sweden

Srinivas, Vivek (author): Stockholms universitet,Institutionen för biokemi och biofysik,Stockholm Univ, Dept Biochem & Biophys, S-10691 Stockholm, Sweden

Högbom, Martin (author): Stockholms universitet,Institutionen för biokemi och biofysik,Stockholm Univ, Dept Biochem & Biophys, S-10691 Stockholm, Sweden

(creator_code:org_t)

2018-06-26
2018
English.
In: Journal of Biological Inorganic Chemistry. - : Springer Science and Business Media LLC. - 0949-8257 .- 1432-1327. ; 23:6, s. 879-886

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Abstract Subject headings

R2-like ligand-binding oxidases contain a dinuclear metal cofactor which can consist either of two iron ions or one manganese and one iron ion, but the heterodinuclear Mn/Fe cofactor is the preferred assembly in the presence of Mn-II and Fe-II in vitro. We have previously shown that both types of cofactor are capable of catalyzing formation of a tyrosine-valine ether cross-link in the protein scaffold. Here we demonstrate that Mn/Fe centers catalyze cross-link formation more efficiently than Fe/Fe centers, indicating that the heterodinuclear cofactor is the biologically relevant one. We further explore the chemical potential of the Mn/Fe cofactor by introducing mutations at the cross-linking valine residue. We find that cross-link formation is possible also to the tertiary beta-carbon in an isoleucine, but not to the secondary beta-carbon or tertiary gamma-carbon in a leucine, nor to the primary beta-carbon of an alanine. These results illustrate that the reactivity of the cofactor is highly specific and directed.

By the author/editor: Griese, Julia J.; Branca, Rui M. M ...; Srinivas, Vivek; Högbom, Martin

About the subject

NATURAL SCIENCES: NATURAL SCIENCES; and Biological Scien ...; and Structural Biolo ...

By the university: Stockholm University; Uppsala University; Karolinska Institutet

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