Multifunctional Two-Dimensional Metal-Organic Frameworks for Radionuclide Sequestration and Detection

Robert G. Surbella, Dallas D. Reilly, Michael A. Sinnwell, Bruce K. McNamara, Lucas E. Sweet, Jon M. Schwantes, Praveen K. Thallapally

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

Abstract

Two lanthanide-containing porous coordination polymers, [Ln2(bpdc)6(phen)2]·nH2O (1) and [Ln2(bpdc)6(terpy)2]·3H2O (2) (Ln = Pr, Nd, or Sm-Dy; bpdc: 2,2′-bipyridine-5,5′-dicarboxylic acid; phen: 1,10-phenanthroline; and terpy: 2,2′:6′,2″-terpyridine), have been hydrothermally synthesized and structurally characterized by powder and single-crystal X-ray diffraction. Crystallographic analyses reveal that compounds 1 and 2 feature Ln3+-containing dimeric nodes that form a porous two-dimensional (2D) and nonporous three-dimensional (3D) framework, respectively. Each material is stable in aqueous media between pH 3 and 10 and exhibits modest thermal stability up to ∼400 °C. Notably, a portion of the phen and bpdc ligands in 1 can be removed thermally, without compromising the crystal structure, causing the surface area and pore volume to increase. The optical properties of 1 and 2 with Gd3+, Sm3+, Tb3+, and Eu3+ are explored in the solid state using absorbance, fluorescence, and lifetime spectroscopies. The analyses reveal a complex blend of metal and ligand emission in the materials containing Sm3+ and Tb3+, while those featuring Eu3+ are dominated by intense metal-based emission. Compound 1 with Eu3+ shows promise for the capture and detection of the uranyl cation (UO2)2+ from aqueous media. In short, uranyl capture is observed at pH 4, and the adsorption thereof is detectable via vibrational and fluorescence spectroscopies and colorimetrically as the off-white color of 1 turns yellow with uptake. Finally, both 1 and 2 with Eu3+ produce bright red emission upon irradiation with Cu Kα X-ray radiation (8.04 keV) and are candidate materials for applications in solid-state scintillation.

Original languageEnglish (US)
Pages (from-to)45696-45707
Number of pages12
JournalACS Applied Materials and Interfaces
Volume13
Issue number38
DOIs
StatePublished - Sep 29 2021

All Science Journal Classification (ASJC) codes

  • General Materials Science

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