4.8 Article

Nucleotide-Selective Templated Self-Assembly of Nanoreactors under Dissipative Conditions

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 49, Pages 22223-22229

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202010199

Keywords

amphiphiles; molecular recognition; network reactivity; self-assembly; systems chemistry

Funding

  1. European Commission [MSCA 657486]
  2. Italian Ministry of Education and Research [2017E44A9P]
  3. University of Padova [CPDA155454]

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Nature adopts complex chemical networks to finely tune biochemical processes. Indeed, small biomolecules play a key role in regulating the flux of metabolic pathways. Chemistry, which was traditionally focused on reactions in simple mixtures, is dedicating increasing attention to the network reactivity of highly complex synthetic systems, able to display new kinetic phenomena. Herein, we show that the addition of monophosphate nucleosides to a mixture of amphiphiles and reagents leads to the selective templated formation of self-assembled structures, which can accelerate a reaction between two hydrophobic reactants. The correct matching between nucleotide and the amphiphile head group is fundamental for the selective formation of the assemblies and for the consequent up-regulation of the chemical reaction. Transient stability of the nanoreactors is obtained under dissipative conditions, driven by enzymatic dephosphorylation of the templating nucleotides. These results show that small molecules can play a key role in modulating network reactivity, by selectively templating self-assembled structures that are able to up-regulate chemical reaction pathways.

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