4.6 Article

An innovative trimetallic-MOF mediated catalytic cleavage activity of FAM tagged Ag10/T-rich DNAzyme as an ultra-sensitive and selective fluorescent biosensor for subsequent recognition of Ag+ and Hg2+ ions

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ELSEVIER SCIENCE SA
DOI: 10.1016/j.jphotochem.2022.113901

关键词

Trimetallic-MOF; DNAzyme; Silver; Mercury; Fluorescence; Biosensor

资金

  1. Selective Excellence Research Initiative Fund SRMIST-2021 from the Department of Chemistry, SRM Institute of Science and Technology, Tamil Nadu, India

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In this study, a biochemical sensing platform was developed using a fluorescent probe and a Trimetallic-MOF for specific and sensitive recognition of Ag+ and Hg2+ ions. The detection was achieved through catalytic cleavage of DNAzyme and the FRET mechanism, resulting in low detection limits and satisfactory recovery in water samples.
In this work, specific and sensitive recognition of the dual metal ions (Ag+ & Hg2+) through the FAM tagged Ag10/T-rich DNAzyme mediated Trimetallic-MOF (Ni/Zn with K-3[Co (CN)(6)]) as a biochemical sensing platform. Interestingly, the fluorescence probe of the FAM tagged specific Ag10/T-rich DNAzyme, and the Trimetallic-MOF demonstrated excellent analytical response towards subsequent recognition of the Ag+ & Hg2+ ions compared to the other coexisting targets. More precisely, the silver enzyme oligomer (EO) and FAM tagged thymine rich substrate oligomer (SO) were hybridized to form the Ag10/T-rich DNAzyme structure. When the Ag+ ion is induced into the Trimetallic-MOF with the FAM tagged Ag10/T-rich DNAzyme complex caused higher efficient internal catalytic cleavage at RNA site of FAM tagged substrate oligomer (SO). The released FAM tagged T-rich SO sequence was adsorbed on the Trimetallic-MOF surface through pi-pi stacking and electrostatic interactions, which diminished (Turn-OFF) the fluorescent signal. Surprisingly, the subsequent addition of the Hg2+ ions into the above-quenched system (Trimetallic-MOF/cleaved FAM tagged SO, and EO with Ag+) resulted in an enhancement of the fluorescence intensity (Turn-ON) due to the creation of the double-strand structure (T-Hg2+- T). By utilizing this sensor, susceptible and discriminating recognition of the Ag+ and Hg2+ ions is attained through the subsequent processes of catalytic cleavage of the DNAzyme and the FRET mechanism. As a result, the proposed biosensor achieved low detection limits of Ag+ (0.29 nM) and Hg2+ (0.10 nM), respectively. The utility of the developed fluorescence biosensor was established due to the subsequent recognition of the Ag+ and Hg2+ in actual water samples with satisfactory regaining and good reproducibility.

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