Enhanced Chemical Synthesis at Soft Interfaces: A Universal Reaction-Adsorption Mechanism in Microcompartments

Ali Fallah-Araghi (1) , Kamel Meguellati (1) , Jean-Christophe Baret (2) , Abdeslam El Harrak (3) , Thomas Mangeat (3) , Martin Karplus (1, 4) , Sylvain Ladame (1, 5) , Carlos M. Marques (6) , Andrew D. Griffiths (7, 1)

1 ISIS - Institut de Science et d'ingénierie supramoléculaires
2 MPIDS - Max Planck Institute for Dynamics and Self-Organization
3 RainDance Technologies, Inc.
4 Harvard University
5 Department of Bioengineering [Imperial College London]
6 ICS - Institut Charles Sadron
7 ESPCI Paris - Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris

A bimolecular synthetic reaction (imine synthesis) was performed compartmentalized in micrometerdiameter emulsion droplets. The apparent equilibrium constant (Keq) and apparent forward rate constant (k1) were both inversely proportional to the droplet radius. The results are explained by a noncatalytic reaction-adsorption model in which reactants adsorb to the droplet interface with relatively low binding energies of a few kBT, react and diffuse back to the bulk. Reaction thermodynamics is therefore modified by compartmentalization at the mesoscale—without confinement on the molecular scale—leading to a universal mechanism for improving unfavorable reactions.

Domaines: Physique [physics]

Ali Fallah-Araghi, Kamel Meguellati, Jean-Christophe Baret, Abdeslam El Harrak, Thomas Mangeat, et al.. Enhanced Chemical Synthesis at Soft Interfaces: A Universal Reaction-Adsorption Mechanism in Microcompartments. Physical Review Letters, 2014, 112 (028301), pp.0283301(1-5). ⟨10.1103/PhysRevLett.112.028301⟩. ⟨hal-01122849⟩