Control of biocatalytic transformations by programmed DNA assemblies

Ronit Freeman, Etery Sharon, Carsten Teller, Itamar Willner*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

25 Scopus citations

Abstract

This study demonstrates the self-assembly of inhibitor/enzyme-tethered nucleic acid fragments or enzyme I-, enzyme II-modified nucleic acids into functional nanostructures that lead to the controlled inhibition of the enzyme or the activation of an enzyme cascade. In one system, the anti-cocaine aptamer subunits are modified with monocarboxy methylene blue (MB+) as the inhibitor and with choline oxidase (ChOx). The cocaine-induced self-assembly of the aptamer subunits complex results in the inhibition of ChOx by MB +. In a further configuration, two nucleic acids of limited complementarity are functionalized at their 3′ and 5′ ends with glucose oxidase (GOx) and horseradish peroxidase (HRP), respectively, or with MB+ and ChOx. In the presence of a target DNA sequence, synergistic complementary base-pairing occurs, thus leading to stable supramolecular Yshaped nanostructures of the nucleic acid units. A GOx/HRP bienzyme cascade or the programmed inhibition of ChOx by MB+ is demonstrated in the resulting nucleic acid nanostructures. A quantitative theoretical model that describes the nucleic acid assemblies and that results in the inhibition of ChOx by MB+ or in the activation of the GOx/HRP cascade, respectively, is provided.

Original languageEnglish
Pages (from-to)3690-3698
Number of pages9
JournalChemistry - A European Journal
Volume16
Issue number12
DOIs
StatePublished - 22 Mar 2010

Keywords

  • Aptamers
  • Cocaine
  • DNA
  • Enzymes
  • Inhibitors

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