Robustness, Entrainment, and Hybridization in Dissipative Molecular Networks, and the Origin of Life

Brian J. Cafferty, Albert S. Y. Wong, Sergey N. Semenov, Lee Belding, Samira Gmur, Wilhelm T. S. Huck, George M. Whitesides*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

47 Citations (Scopus)

Abstract

How simple chemical reactions self-assembled into complex, robust networks at the origin of life is unknown. This general problem-self-assembly of dissipative molecular networks-is also important in understanding the growth of complexity from simplicity in molecular and biomolecular systems. Here, we describe how heterogeneity in the composition of a small network of oscillatory organic reactions can sustain (rather than stop) these oscillations, when homogeneity in their composition does not. Specifically, multiple reactants in an amide-forming network sustain oscillation when the environment (here, the space velocity) changes, while homogeneous networks-those with fewer reactants-do not. Remarkably, a mixture of two reactants of different structure-neither of which produces oscillations individually-oscillates when combined. These results demonstrate that molecular heterogeneity present in mixtures of reactants can promote rather than suppress complex behaviors.

Original languageEnglish
Pages (from-to)8289-8295
Number of pages7
JournalJournal of the American Chemical Society
Volume141
Issue number20
Early online date30 Apr 2019
DOIs
Publication statusPublished - 22 May 2019

Funding

We thank Dr. Dmitry Zubarev for assistance on earlier versions of this manuscript. This work was supported by an award (290364) from the Simons Foundations. A.S.Y.W. is supported by funding from The Netherlands Organization for Scientific Research (NWO, Rubicon program, project no. 019.172EN.017). L.B. acknowledges fellowship support from NSERC Canada.

All Science Journal Classification (ASJC) codes

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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