Positive Effects of ATP on G-Quadruplex-Hemin DNAzyme-Mediated Reactions

Abstract

Some G-quadruplex-hemin complexes can be used as peroxidase-mimicking DNAzymes, catalyzing H(2)O(2)-mediated reactions such as the oxidation of 2,2'-azinobis (3-ethylbenzothiozoline)-6-sulfonic acid (ABTS) by H(2)O(2). However, some challenges, for example, the relatively low catalytic activity and the disproportionation of the reaction product ABTS*(+), may seriously restrict further development and applications of these complexes. Here, we demonstrated the positive effect of adenosine triphosphate (ATP) on G-quadruplex-hemin DNAzyme-mediated catalytic reactions. The presence of ATP not only improved the catalytic activity of G-quadruplex-hemin DNAzymes, but also inhibited the disproportionation of ABTS*(+). These observations may improve the performance of existing G-quadruplex-hemin DNAzyme-based chemical sensors, for example, the Ag(+)-detection method that uses G-quadruplex-hemin DNAzymes, and widen the application range of G-quadruplex-hemin DNAzymes. We also demonstrated that the phosphate groups, nucleobase, and sugar of ATP determine the reaction-promoting ability of ATP. These observations may be helpful in the design of highly efficient enhancers for G-quadruplex-hemin DNAzymes.

Incorporating ATP into biomimetic catalysts for realizing exceptional enzymatic performance over a broad temperature range

“…However, it is well known that ATP is not only considered to be the ubiquitous energy currency of life, 35 but is also well known to form charge transfer complexes with aromatic molecules and to participate in free radical redox chemistry. [36][37][38][39] For instance, the positive effects of ATP on ribonucleotide reductase-mediated catalytic reactions have been reported. 37 In addition, ATP could bind to an in vitro-selected Enzymatic performance of ATP over a broad temperature range Y Lin et al 27-base anti-ATP aptamer with high affinity and could induce the aptamer to undergo a conformational change from random coil to tertiary structure.…”

“…Inspired by the recent reports from Monchaud and colleagues 35 and Kong et al, 39 we assumed that ATP could also be used as an effective modulator to inhibit disproportionation and stabilize cationic free radical ABTS Áþ at high temperature. 35,39 To evaluate the feasibility of our presumption, we explored the effects of ATP concentration on the thermal stability of the reaction product in the presence of 60 mM H 2 O 2 . As shown in Figures 3c and d, the disproportionation of ABTS Á þ is gradually inhibited with increasing ATP concentration.…”

Improved method for chemiluminescent determination of peroxidase-mimicking DNAzyme activity

“…It should be noted that ABTS is not an ideal substrate because ABTS + forming on the oxidation of ABTS is not a stable compound and quickly disproportionates with the production of colorless compounds [26,27]. Of the above-mentioned methods, the CL method, which is based on PMDNAzyme-catalyzed oxidation of luminol with a generation of light, is the most sensitive [22][23][24].…”

DNAzyme based gap-LCR detection of single-nucleotide polymorphism

“…However, the NADH-dependent thermal stable Taq DNA ligase which had been commonly used in the original LCR reaction was excluded from our method because the co-enzyme NADH of the ligase would interfere with the oxidation reaction catalyzed by the DNAzyme (data not shown). An ATP-dependent thermal stable DNA ligase 91N (NEB) was applied in our system since ATP is not only compatible with our G-quadruplex DNAzyme but also helpful to the colorimetric reaction catalyzed by DNAzyme using ABTS as substrate (Kong et al, 2010). Under optimized condition, trace amount of mutant b-globin gene were successfully amplified by our probes, which indicate the additional DNAzyme sequence on the probe would not interfere the Gap-LCR amplification (Lane 4, Fig.…”