Construction of Molecular Sensing and Logic Systems Based on Site-Occupying Effect-Modulated MOF–DNA Interaction

Abstract

Interactions between metal−organic frameworks (MOFs) and nucleic acids are of great importance in molecular assembly. However, current MOF−nucleic acid interactions lack diversity and are normally realized in an uncontrollable manner. Herein, the interaction of zirconium-based MOFs (Zr-MOFs) with nucleic acids is enabled by the formation of Zr−O−P bonds and further manipulated by a phosphate-induced site-occupying effect. Covering Zr ions in clusters of MOFs with phosphates impedes the formation of Zr−O−P bonds with nucleic acids, rendering the MOF−nucleic acid interaction tunable and stimulus-responsive. Notably, the experimental results demonstrate that various phosphates, Zr-MOFs, and nucleic acids can all be adopted in the tunable interaction. On the basis of these findings, fluorescent DNA and typical Zr-MOFs are proposed as functional probe−quencher pairs to establish molecular sensing and logic systems. Accordingly, alkaline phosphatase and inorganic pyrophosphatase can be quantified simultaneously, and the overall relation of different phosphates and phosphatases is facilely displayed. The work provides a general strategy for modulating MOF−nucleic acid interactions, which is conducive to the development of molecular intelligent systems.

CaZnO-based nanoghosts for the detection of ssDNA, pCRISPR and recombinant SARS-CoV-2 spike antigen and targeted delivery of doxorubicin

“…In order to analyze the pCRISPR and ssDNA interactions with the NGs, these genetic materials were exposed to varying concentrations of NGs. Quenching of the fluorescence emission of the NGs-porphyrin was expected because of the presence of similar interaction of the Zn(Ca)–O–P bonds as recently shown by Yu et al in the presence of Zr-MOF and ssDNA ( Yu et al, 2020a ). The results of the fluorescence emission spectra showed that after loading the ssDNA on the NGs-porphyrin, the fluorescence emission decayed significantly ( Fig.…”

Dual Intrareticular Oxidation of Mixed-Ligand Metal–Organic Frameworks for Stepwise Electrochemiluminescence

“…Metal–organic frameworks (MOFs) can be finely tuned to exhibit unique properties by careful design of the metallic units and organic linkers . In particular, the mixed-ligand strategy with multiple building units has been proven to be a viable approach for synthesizing functionally tunable MOFs .…”

“…Metal−organic frameworks (MOFs) can be finely tuned to exhibit unique properties by careful design of the metallic units and organic linkers. 15 In particular, the mixed-ligand strategy with multiple building units has been proven to be a viable approach for synthesizing functionally tunable MOFs. 16 In contrast to single-ligand MOFs (s-MOFs), mixed-ligand MOFs (m-MOFs) enable multiple functionalities by integration of various ligands and have been broadly applied in different fields.…”

Logic devices based on nucleic acid self‐assembly

“…Nanotechnology has offered exciting opportunities in the construction of multiscale logic gate networks from single molecules to customized nanostructures that can process information and realize predetermined functions. [8][9][10] With the rapid development of DNA and RNA nanotechnology, nucleic acid strands and assemblies have provided intriguing strategies for the design and construction of logic devices. For nucleic acid molecules, only approximately 50 atoms (one base pair) are needed to store one 1-bit information, which exhibits outstanding capability potential for miniaturizing information storage devices.…”