Redox cycling and kinetic analysis of single molecules of solution-phase nitrite reductase

Proc Natl Acad Sci U S A. 2011 Oct 18;108(42):17269-74. doi: 10.1073/pnas.1113572108. Epub 2011 Oct 3.

Abstract

Single-molecule measurements are a valuable tool for revealing details of enzyme mechanisms by enabling observation of unsynchronized behavior. However, this approach often requires immobilizing the enzyme on a substrate, a process which may alter enzyme behavior. We apply a microfluidic trapping device to allow, for the first time, prolonged solution-phase measurement of single enzymes in solution. Individual redox events are observed for single molecules of a blue nitrite reductase and are used to extract the microscopic kinetic parameters of the proposed catalytic cycle. Changes in parameters as a function of substrate concentration are consistent with a random sequential substrate binding mechanism.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Alcaligenes / enzymology
  • Alcaligenes / genetics
  • Amino Acid Substitution
  • Bacterial Proteins / chemistry
  • Bacterial Proteins / genetics
  • Bacterial Proteins / metabolism
  • Copper / chemistry
  • Fluorescence Resonance Energy Transfer
  • Kinetics
  • Microfluidic Analytical Techniques
  • Models, Molecular
  • Mutagenesis, Site-Directed
  • Nitrite Reductases / chemistry*
  • Nitrite Reductases / genetics
  • Nitrite Reductases / metabolism*
  • Oxidation-Reduction
  • Protein Structure, Quaternary
  • Recombinant Proteins / chemistry
  • Recombinant Proteins / genetics
  • Recombinant Proteins / metabolism
  • Solutions

Substances

  • Bacterial Proteins
  • Recombinant Proteins
  • Solutions
  • Copper
  • Nitrite Reductases