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Ribonucleotide reductases

A Jordan1, P Reichard

  • 1Department of Genetics and Microbiology, Faculty of Sciences, Autonomous University of Barcelona, Bellaterra, Spain.

Annual Review of Biochemistry
|October 6, 1998
PubMed
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Ribonucleotide reductases are essential for DNA replication. The study reveals structural insights into class I enzymes, suggesting a common evolutionary origin for all reductase classes.

Area of Science:

  • Biochemistry
  • Molecular Biology
  • Enzymology

Background:

  • Ribonucleotide reductases (RNRs) are crucial enzymes that catalyze the conversion of ribonucleotides to deoxyribonucleotides, the essential building blocks for DNA synthesis.
  • Three distinct classes of RNRs (Class I, II, and III) exist, each utilizing unique cofactor-dependent mechanisms involving protein free radicals to activate the substrate.
  • Class I RNRs employ a tyrosyl radical and an iron-oxygen center, Class II RNRs utilize adenosylcobalamin, and Class III RNRs generate a glycyl radical using S-adenosylmethionine and an iron-sulfur cluster.

Purpose of the Study:

  • To elucidate the structural basis of catalysis and allosteric regulation in Class I Ribonucleotide Reductases.
  • To investigate the mechanism of radical transfer between subunits in Class I RNRs.
  • To explore the evolutionary relationships and common origins of the different classes of RNRs.

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Main Methods:

  • X-ray crystallography was used to determine the structure of the Class I Escherichia coli RNR, including complexes with substrate and allosteric effectors.
  • Site-directed mutagenesis experiments were conducted to probe the mechanism of radical transfer and enzyme function.

Main Results:

  • The X-ray structure of the Class I E. coli RNR confirmed existing models of its catalytic and allosteric mechanisms.
  • The determined structure revealed significant protein mobility during catalysis, suggesting a dynamic mechanism.
  • Experiments indicated a mechanism for radical transfer between enzyme subunits.

Conclusions:

  • The structural and mechanistic insights into Class I RNRs provide a detailed understanding of DNA precursor synthesis.
  • Despite mechanistic differences, conserved residues and common catalytic/allosteric strategies suggest a shared evolutionary origin for all RNR classes.
  • The presence of multiple RNR genes in some organisms remains an area for further investigation.