Capture Instead of Release: Defect-Modulated Radionuclide Leaching Kinetics in Metal-Organic Frameworks.

Autor: Park KC; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Martin CR; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Leith GA; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Thaggard GC; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Wilson GR; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Yarbrough BJ; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Maldeni Kankanamalage BKP; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Kittikhunnatham P; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Mathur A; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Jatoi I; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Manzi MA; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Lim J; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Lehman-Andino I; Savannah River National Laboratory, Aiken, South Carolina 29808, United States., Hernandez-Jimenez A; Savannah River National Laboratory, Aiken, South Carolina 29808, United States., Amoroso JW; Savannah River National Laboratory, Aiken, South Carolina 29808, United States., DiPrete DP; Savannah River National Laboratory, Aiken, South Carolina 29808, United States., Liu Y; Department of Materials Science and Engineering, University of Florida, Gainesville, Florida 32611, United States., Schaeperkoetter J; Kazuo Inamori School of Engineering, Alfred University, Alfred, New York 14802, United States., Misture ST; Kazuo Inamori School of Engineering, Alfred University, Alfred, New York 14802, United States., Phillpot SR; Department of Materials Science and Engineering, University of Florida, Gainesville, Florida 32611, United States., Hu S; Pacific Northwest National Laboratory, Richland, Washington 99352, United States., Li Y; Pacific Northwest National Laboratory, Richland, Washington 99352, United States., Leydier A; Commissariat à l'Énergie Atomique (CEA), DES, ISEC, DMRC, University Montpellier, Marcoule, BP 17171, 30207 Bagnols-sur-Cèze Cedex, France., Proust V; Commissariat à l'Énergie Atomique (CEA), DES, ISEC, DMRC, University Montpellier, Marcoule, BP 17171, 30207 Bagnols-sur-Cèze Cedex, France., Grandjean A; Commissariat à l'Énergie Atomique (CEA), DES, ISEC, DMRC, University Montpellier, Marcoule, BP 17171, 30207 Bagnols-sur-Cèze Cedex, France., Smith MD; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States., Shustova NB; Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2022 Sep 07; Vol. 144 (35), pp. 16139-16149. Date of Electronic Publication: 2022 Aug 26.
DOI: 10.1021/jacs.2c06905
Abstrakt: Comparison of defect-controlled leaching-kinetics modulation of metal-organic frameworks (MOFs) and porous functionalized silica-based materials was performed on the example of a radionuclide and radionuclide surrogate for the first time, revealing an unprecedented readsorption phenomenon. On a series of zirconium-based MOFs as model systems, we demonstrated the ability to capture and retain >99% of the transuranic 241 Am radionuclide after 1 week of storage. We report the possibility of tailoring radionuclide release kinetics in MOFs through framework defects as a function of postsynthetically installed organic ligands including cation-chelating crown ether-based linkers. Based on comprehensive analysis using spectroscopy (EXAFS, UV-vis, FTIR, and NMR), X-ray crystallography (single crystal and powder), and theoretical calculations (nine kinetics models and structure simulations), we demonstrated the synergy of radionuclide integration methods, topological restrictions, postsynthetic scaffold modification, and defect engineering. This combination is inaccessible in any other material and highlights the advantages of using well-defined frameworks for gaining fundamental knowledge necessary for the advancement of actinide-based material development, providing a pathway for addressing upcoming challenges in the nuclear waste administration sector.
Databáze: MEDLINE