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Enhanced Chemical Synthesis at Soft Interfaces: A Universal Reaction-Adsorption Mechanism in Microcompartments
Abstract
A bimolecular synthetic reaction (imine synthesis) was performed compartmentalized in micrometer-diameter 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.
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Cites
On the origin of genomes and cells within inorganic compartments
Koonin, E. V., & Martin, W. (2005) · Trends in Genetics · doi:10.1016/j.tig.2005.09.006 · Cited by 406
From Prelife to Life: How Chemical Kinetics Become Evolutionary Dynamics
Chen, I. A., & Nowak, M. A. (2012) · Accounts of Chemical Research · doi:10.1021/ar2002683 · Cited by 50
Cited by
Accelerated Reaction Kinetics in Microdroplets: Overview and Recent Developments
Wei, Z., Li, Y., Cooks, R. G., & Yan, X. (2020) · Annual Review of Physical Chemistry · doi:10.1146/annurev-physchem-121319-110654 · Cited by 631
Organic Reactions in Microdroplets: Reaction Acceleration Revealed by Mass Spectrometry
Yan, X., Bain, R. M., & Cooks, R. G. (2016) · Angewandte Chemie International Edition · doi:10.1002/anie.201602270 · Cited by 583
Molecular reactions at aqueous interfaces
Ruiz-Lopez, M. F., Francisco, J. S., Martins-Costa, M. T. C., & Anglada, J. M. (2020) · Nature Reviews Chemistry · doi:10.1038/s41570-020-0203-2 · Cited by 411
Weber, C. A., Zwicker, D., Jülicher, F., & Lee, C. F. (2019) · Reports on Progress in Physics · doi:10.1088/1361-6633/ab052b · Cited by 298
Abiotic production of sugar phosphates and uridine ribonucleoside in aqueous microdroplets
Nam, I., Lee, J. K., Nam, H. G., & Zare, R. N. (2017) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1714896114 · Cited by 262
Metadata
- Authors
- Fallah-Araghi, A., Meguellati, K., Baret, J.-C., Harrak, A. E., Mangeat, T., Karplus, M., Ladame, S., Marques, C. M., & Griffiths, A. D.
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2014-01-13
- Volume
- 112
- Issue
- 2
- Pages
- 028301-028301
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W2008615905
- Cited by
- 301
- References
- 2
- FWCI
- 10.43
- Type
- journal article
- Language
- en
- Open access
- closed
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- Fallah-Araghi, A., Meguellati, K., Baret, J.-C., Harrak, A. E., Mangeat, T., Karplus, M., Ladame, S., Marques, C. M., & Griffiths, A. D. (2014). Enhanced Chemical Synthesis at Soft Interfaces: A Universal Reaction-Adsorption Mechanism in Microcompartments. Physical Review Letters. https://doi.org/10.1103/physrevlett.112.028301
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