Force-activated reactivity switch in a bimolecular chemical reaction

Nat Chem. 2009 Jun;1(3):236-42. doi: 10.1038/nchem.207. Epub 2009 May 10.

Abstract

The effect of mechanical force on the free-energy surface that governs a chemical reaction is largely unknown. The combination of protein engineering with single-molecule force-clamp spectroscopy allows us to study the influence of mechanical force on the rate at which a protein disulfide bond is reduced by nucleophiles in a bimolecular substitution reaction (S(N)2). We found that cleavage of a protein disulfide bond by hydroxide anions exhibits an abrupt reactivity 'switch' at ∼500 pN, after which the accelerating effect of force on the rate of an S(N)2 chemical reaction greatly diminishes. We propose that an abrupt force-induced conformational change of the protein disulfide bond shifts its ground state, drastically changing its reactivity in S(N)2 chemical reactions. Our experiments directly demonstrate the action of a force-activated switch in the chemical reactivity of a single molecule.

Publication types

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

MeSH terms

  • Amino Acid Substitution
  • Connectin
  • Disulfides / chemistry
  • Hydroxides / chemistry
  • Macromolecular Substances / chemistry*
  • Microscopy, Atomic Force
  • Muscle Proteins / chemistry
  • Protein Engineering
  • Protein Kinases / chemistry
  • Proteins / chemistry
  • Thermodynamics

Substances

  • Connectin
  • Disulfides
  • Hydroxides
  • Macromolecular Substances
  • Muscle Proteins
  • Proteins
  • hydroxide ion
  • Protein Kinases