Methodology to probe subunit interactions in ribonucleotide reductases

Biochemistry. 2008 Dec 9;47(49):13046-55. doi: 10.1021/bi8012559.

Abstract

Ribonucleotide reductases (RNRs) catalyze the conversion of nucleotides to deoxynucleotides, providing the monomeric precursors required for DNA replication and repair. Escherichia coli RNR is a 1:1 complex of two homodimeric subunits, alpha2 and beta2. The interactions between alpha2 and beta2 are thought to be largely associated with the C-terminal 20 amino acids (residues 356-375) of beta2. To study subunit interactions, a single reactive cysteine has been introduced into each of 15 positions along the C-terminal tail of beta2. Each cysteine has been modified with the photo-cross-linker benzophenone (BP) and the environmentally sensitive fluorophore dimethylaminonaphthalene (DAN). Each construct has been purified to homogeneity and characterized by sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE) and electrospray ionization mass spectrometry (ESI-MS). Each BP-beta2 has been incubated with 1 equiv of alpha2 and photolyzed, and the results have been analyzed quantitatively by SDS-PAGE. Each DAN-beta2 was incubated with a 50-fold excess of alpha2, and the emission maximum and intensity were measured. A comparison of the results from the two sets of probes reveals that sites with the most extensive cross-linking are also associated with the greatest changes in fluorescence. Titration of four different DAN-beta2 variants (351, 356, 365, and 367) with alpha2 gave a K(d) approximately 0.4 microM for subunit interaction. Disruption of the interaction of the alpha2-DAN-beta2 complex is accompanied by a decrease in fluorescence intensity and can serve as a high-throughput screen for inhibitors of subunit interactions.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • 2-Naphthylamine / chemistry
  • Benzophenones / chemistry
  • Biotechnology*
  • Cross-Linking Reagents / chemistry
  • Cysteine / chemistry
  • Cysteine / genetics
  • Cysteine / metabolism
  • Electron Spin Resonance Spectroscopy
  • Electrophoresis, Polyacrylamide Gel
  • Escherichia coli / enzymology*
  • Kinetics
  • Mutation
  • Protein Binding
  • Protein Subunits / chemistry*
  • Protein Subunits / genetics
  • Protein Subunits / metabolism*
  • Ribonucleotide Reductases / chemistry*
  • Ribonucleotide Reductases / genetics
  • Ribonucleotide Reductases / metabolism*
  • Spectrometry, Fluorescence

Substances

  • Benzophenones
  • Cross-Linking Reagents
  • Protein Subunits
  • 2-Naphthylamine
  • Ribonucleotide Reductases
  • Cysteine