Multifunctional two-dimensional metal-organic frameworks for radionuclide sequestration and detection

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

doi:10.1021/acsami.1c11018

Multifunctional two-dimensional metal-organic frameworks for radionuclide sequestration and detection

Journal Article · 29 September 2021 · ACS Applied Materials & Interfaces

DOI:https://doi.org/10.1021/acsami.1c11018· OSTI ID:1829674

^[1]; Reilly, Dallas D. ^[1]; ^[1]; Mcnamara, Bruce K. ^[2]; ^[1]; ^[1]; ^[1]

BATTELLE (PACIFIC NW LAB)
Battelle Washington Office, Washington, D.C.

Two lanthanide containing porous coordination polymers, [Ln2(bpdc)6(phen)2] · nH2O (1) and [Ln2(bpdc)6(terpy)2] · 3H2O (2) (Ln = either 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. The crystallographic analyses reveal compounds 1 and 2 feature Ln3+ containing dimeric nodes that form a porous two-dimensional (2D) and non-porous three-dimensional (3D) framework, respectively. Each material is stable in aqueous media between pH 3-10 and exhibits modest thermal stability to ~400ºC. 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+ were 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+ displayed promise for the capture and detection of the uranyl cation, (UO2)2+, from aqueous media. In short, uranyl capture was observed at pH 4 and the adsorption thereof was detectable via vibrational and fluorescence spectroscopies and colorimetrically as the off-white color of 1 turned yellow with uptake. Finally, both 1 and 2 with Eu3+ produce bright red emission upon irradiation with Cu ka X-ray radiation (8.04 keV) and are candidate materials for applications in solid-state scintillation.

Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1829674

Report Number(s):: PNNL-SA-161938

Journal Information:: ACS Applied Materials & Interfaces, Vol. 13, Issue 38

Country of Publication:: United States

Language:: English

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