Nucleoapzymes: Hemin/G-Quadruplex DNAzyme-Aptamer Binding Site Conjugates with Superior Enzyme-like Catalytic Functions

Eyal Golub, H. Bauke Albada, Wei Ching Liao, Yonatan Biniuri, Itamar Willner

Research output: Contribution to journalArticlepeer-review

201 Scopus citations


A novel concept to improve the catalytic functions of nucleic acids (DNAzymes) is introduced. The method involves the conjugation of a DNA recognition sequence (aptamer) to the catalytic DNAzyme, yielding a hybrid structure termed "nucleoapzyme". Concentrating the substrate within the "nucleoapzyme" leads to enhanced catalytic activity, displaying saturation kinetics. Different conjugation modes of the aptamer/DNAzyme units and the availability of different aptamer sequences for a substrate provide diverse means to design improved catalysts. This is exemplified with (i) The H2O2-mediated oxidation of dopamine to aminochrome using a series of hemin/G-quadruplex-dopamine aptamer nucleoapzymes. All nucleoapzymes reveal enhanced catalytic activities as compared to the separated DNAzyme/aptamer units, and the most active nucleoapzyme reveals a 20-fold enhanced activity. Molecular dynamics simulations provide rational assessment of the activity of the various nucleoapzymes. The hemin/G-quadruplex-aptamer nucleoapzyme also stimulates the chiroselective oxidation of l- vs d-DOPA by H2O2. (ii) The H2O2-mediated oxidation of N-hydroxy-l-arginine to l-citrulline by a series of hemin/G-quadruplex-arginine aptamer conjugated nucleoapzymes.

Original languageEnglish
Pages (from-to)164-172
Number of pages9
JournalJournal of the American Chemical Society
Issue number1
StatePublished - 13 Jan 2016
Externally publishedYes

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© 2015 American Chemical Society.


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