Gated Proton Release during Radical Transfer at the Subunit Interface of Ribonucleotide Reductase.

ABSTRACT: The class Ia ribonucleotide reductase of Escherichia coli requires strict regulation of long-range radical transfer between two subunits, α and β, through a series of redox-active amino acids (Y₁₂₂•[β] ↔ W₄₈?[β] ↔ Y₃₅₆[β] ↔ Y₇₃₁[α] ↔ Y₇₃₀[α] ↔ C₄₃₉[α]). Nowhere is this more precarious than at the subunit interface. Here, we show that the oxidation of Y₃₅₆ is regulated by proton release involving a specific residue, E₅₂[β], which is part of a water channel at the subunit interface for rapid proton transfer to the bulk solvent. An E₅₂Q variant is incapable of Y₃₅₆ oxidation via the native radical transfer pathway or non-native photochemical oxidation, following photosensitizat

SUBMITTER: Cui C 

PROVIDER: S-EPMC7904477 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature