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Mechanistic Insight of Sensing Hydrogen Phosphate in Aqueous Medium by Using Lanthanide(III)-Based Luminescent Probes.

ABSTRACT: The development of synthetic lanthanide luminescent probes for selective sensing or binding anions in aqueous medium requires an understanding of how these anions interact with synthetic lanthanide probes. Synthetic lanthanide probes designed to differentiate anions in aqueous medium could underpin exciting new sensing tools for biomedical research and drug discovery. In this direction, we present three mononuclear lanthanide-based complexes, EuLCl₃ (1), SmLCl₃ (2), and TbLCl₃ (3), incorporating a hexadentate aminomethylpiperidine-based nitrogen-rich heterocyclic ligand L for sensing anion and establishing mechanistic insight on their binding activities in aqueous medium. All these complexes are meticulously studied for their preferential selectivities towards different anions such as HPO₄^2-, SO₄^2-, CH₃COO^-, I^-, Br^-, Cl^-, F^-, NO₃^-, CO₃^2-/HCO₃^-, and HSO₄^- at pH 7.4 in aqueous HEPES (2-[4-(2-hydroxyethyl)piperazin-1-yl]ethanesulfonic acid) buffer. Among the anions scanned, HPO₄^2- showed an excellent luminescence change with all three complexes. Job's plot and ESI-MS support the 1:2 association between the receptors and HPO₄^2-. Systematic spectrophotometric titrations of 1-3 against HPO₄^2- demonstrates that the emission intensities of 1 and 2 were enhanced slightly upon the addition of HPO₄^2- in the range 0.01-1 equiv and 0.01-2 equiv., respectively. Among the three complexes, complex 3 showed a steady quenching of luminescence throughout the titration of hydrogen phosphate. The lower and higher detection limits of HPO₄^2- by complexes 1 and 2 were determined as 0.1-4 mM and 0.4-3.2 mM, respectively, while complex 3 covered 0.2-100 ?M. This concludes that all complexes demonstrated a high degree of sensitivity and selectivity towards HPO₄^2-.

SUBMITTER: Sahoo J

PROVIDER: S-EPMC7824681 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Mechanistic Insight of Sensing Hydrogen Phosphate in Aqueous Medium by Using Lanthanide(III)-Based Luminescent Probes.

Sahoo Jashobanta J Jaiswar Santlal S Chatterjee Pabitra B PB Subramanian Palani S PS Jena Himanshu Sekhar HS

Nanomaterials (Basel, Switzerland) 20201228 1

The development of synthetic lanthanide luminescent probes for selective sensing or binding anions in aqueous medium requires an understanding of how these anions interact with synthetic lanthanide probes. Synthetic lanthanide probes designed to differentiate anions in aqueous medium could underpin exciting new sensing tools for biomedical research and drug discovery. In this direction, we present three mononuclear lanthanide-based complexes, EuLCl3 (1), SmLCl3 (2 ...[more]

PMID: 33379340

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Project description:Flexible metal-organic frameworks offer a route towards high useable hydrogen storage capacities with minimal swings in pressure and temperature via step-shaped adsorption and desorption profiles. Yet, the understanding of hydrogen-induced flexibility in candidate storage materials remains incomplete. Here, we investigate the hydrogen storage properties of a quintessential flexible metal-organic framework, ZIF-7. We use high-pressure isothermal hydrogen adsorption measurements to identify the pressure-temperature conditions of the hydrogen-induced structural transition in ZIF-7. The material displays narrow hysteresis and has a shallow adsorption slope between 100 K and 125 K. To gain mechanistic insight into the cause of the phase transition correlating with stepped adsorption and desorption, we conduct powder neutron diffraction measurements of the D2 gas-dosed structures at conditions across the phase change. Rietveld refinements of the powder neutron diffraction patterns yield the structures of activated ZIF-7 and of the gas-dosed material in the dense and open phases. The structure of the activated phase of ZIF-7 is corroborated by the structure of the activated phase of the Cd congener, CdIF-13, which we report here for the first time based on single crystal X-ray diffraction measurements. Subsequent Rietveld refinements of the powder patterns for the gas-dosed structure reveal that the primary D2 adsorption sites in the dense phase form D2-arene interactions between adjacent ligands in a sandwich-like adsorption motif. These sites are prevalent in both the dense and the open structure for ZIF-7, and we hypothesize that they play an important role in templating the structure of the open phase. We discuss the implications of our findings for future approaches to rationally tune step-shaped adsorption in ZIF-7, its congeners, and flexible porous adsorbents in general. Lastly, important to the application of flexible frameworks, we show that pelletization of ZIF-7 produces minimal variation in performance.

Dataset Information

Mechanistic Insight of Sensing Hydrogen Phosphate in Aqueous Medium by Using Lanthanide(III)-Based Luminescent Probes.

Publications

Mechanistic Insight of Sensing Hydrogen Phosphate in Aqueous Medium by Using Lanthanide(III)-Based Luminescent Probes.

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