Experimental and theoretical validations of a one-pot sequential sensing of Hg
Hg(2+) and biothiols detection
Metal–organic framework
Molecular simulation
Sequential sensing
Journal
Talanta
ISSN: 1873-3573
Titre abrégé: Talanta
Pays: Netherlands
ID NLM: 2984816R
Informations de publication
Date de publication:
01 Apr 2020
01 Apr 2020
Historique:
received:
06
08
2018
revised:
21
11
2019
accepted:
25
11
2019
entrez:
29
1
2020
pubmed:
29
1
2020
medline:
27
10
2020
Statut:
ppublish
Résumé
A zwitterionic three-dimensional (3D) metal-organic framework (MOF) of {[Cu(Cdcbp)(bipy)]·4H
Identifiants
pubmed: 31987206
pii: S0039-9140(19)31229-9
doi: 10.1016/j.talanta.2019.120596
pii:
doi:
Substances chimiques
Fluorescent Dyes
0
Metal-Organic Frameworks
0
Sulfhydryl Compounds
0
Copper
789U1901C5
Mercury
FXS1BY2PGL
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
120596Informations de copyright
Copyright © 2019 Elsevier B.V. All rights reserved.
Déclaration de conflit d'intérêts
Declaration of competing interest MOFs have shown rich potential as sensors for metal ions, small organics, and biomolecules. However, to the best of our knowledge, utilizing DNA@MOF hybrid as biosensing platform for the simultaneous detection of Hg(2+) and biothiols, both of whom are biologically relevant, has not been revealed. We report in this manuscript a Cu(II)-based 3D MOF which can absorb FAM-labeled T-rich P-DNA to give a P-DNA@MOF hybrid and quench the FAM fluorescence (off-state). The resultant P-DNA@MOF system, in turn, can be employed for the analysis of Hg(2+) triggered by the formation of hairpin-like T-Hg(2+)-T structure, followed by its detachment from the MOF and accompanied by the recovery of FAM fluorescence (on-state). A subsequent competitive Hg–S coordination between Hg(2+) and biothiols (Cys, GSH, and Hcy) serves to liberate the P-DNA from the T-Hg(2+)-T duplex, and resorbed by the MOF to quench the FAM fluorescence again (off-state). Through the fluorescence “off-on-off” cycle, we thus accomplished, for the first time, the simultaneous detection of Hg(2+) and biothiols by a DNA@MOF platform. The detection mechanism was further confirmed by circular dichroism (CD), fluorescence anisotropy (FA), binding constant, as well as the energy and structural simulations. While Hg(2+) and biothiols have their individual roles to play in the biological systems, a sequential dual sensing of the two may serve to counter-proof the presence of each other and provide additional diagnostic accuracy. With the good recovery efficiency of Hg(2+) and Hcy in environmental water and in serum, we assume that such a sequential dual sensing of two biologically relevant, yet completely different substrates may find potential application in the diagnosis of related diseases, such as Parkinson's disease.