Experimental and Theoretical Elucidation of the Luminescence Quenching Mechanism in Highly Efficient Hg 2+ and Sulfadiazine Sensing by Ln-MOF.
Xiaolin YuDmitry I PavlovAlexey A RyadunKonstantin A KovalenkoTatiana Y GuselnikovaEnrico BenassiAndrei S PotapovVladimir Petrovich FedinPublished in: Angewandte Chemie (International ed. in English) (2024)
Heavy metal ions and antibiotic contamination have become a major environmental concern worldwide. The development of efficient recognition strategies of these pollutants at ultra-low concentrations in aqueous solutions as well as the elucidation of the intrinsic sensing mechanism are challenging tasks. In this work, unique luminescent Ln-MOF materials (NIIC-3-Ln) were assembled by rational ligand design. Among them, NIIC-3-Tb demonstrated highly selective luminescence quenching response toward Hg 2+ and sulfadiazine (SDI) at subnanomolar concentrations in less than 7 s. In addition, a Hg 2+ sensing mechanism through chelation was proposed on the basis of single-crystal X-ray diffraction analysis and Hg 2+ adsorption study. The interaction mechanism of NIIC-3-Tb with SDI was revealed using a newly developed approach involving a (TD-)DFT based quantification of the charge transfer of a MOF-analyte supramolecular complex model in the ground and excited states. Effect of ultrasonic treatment on the surface morphology important for MOF sensing performance was revealed by gas adsorption experiments. The presented results indicate that NIIC-3-Ln is not only an advanced sensing material for the efficient detection of Hg 2+ and SDI at ultra-low concentrations, but also opens up a new approach to study the sensing mechanism at the molecular level at ultra-low concentrations.
Keyphrases
- aqueous solution
- energy transfer
- highly efficient
- high resolution
- metal organic framework
- quantum dots
- fluorescent probe
- heavy metals
- mycobacterium tuberculosis
- living cells
- magnetic resonance imaging
- mass spectrometry
- computed tomography
- magnetic resonance
- working memory
- health risk
- drinking water
- climate change
- combination therapy
- molecular docking
- molecular dynamics
- ionic liquid