Synthesis, thermogravimetric analysis and enthalpy determination of lanthanide β-diketonates
Author:
Shahbazi Shayan1, Oldham C. J.1, Mullen Austin D.1, Auxier II John D.123, Hall Howard L.123
Affiliation:
1. Department of Nuclear Engineering, 301 Middle Dr., Pasqua Nuclear Engineering Building , University of Tennessee , Knoxville, TN 37996 , USA 2. Radiochemistry Center of Excellence, 1508 Middle Dr., Ferris Hall, University of Tennessee , Knoxville, TN 37996 , USA 3. Institute for Nuclear Security, 1640 Cumberland Ave. Howard Baker Jr. Center for Public Policy, University of Tennessee , Knoxville, TN 37996 , USA
Abstract
Abstract
This work reports thermodynamic characterizations of lanthanide β-diketonates for use in nuclear fission product separation. Adsorption and sublimation enthalpies have been shown to be linearly correlated, therefore there is motivation to determine sublimation thermodynamics. An isothermal thermogravimetric analysis method is employed on fourteen lanthanide chelates for the ligands 2,2,6,6-tetramethyl-3,5-heptanedione and 6,6,7,7,8,8,8-heptafluoro-2,2-dimethyl-3,5-octanedione to determine sublimation enthalpies. No linear trend is seen across the series; values show a cyclical nature, possibly indicating a greater influence of chemisorption for some complexes and less of a role of physisorption in dictating adsorption differences between lanthanides in the same series. This is in line with previous reports in terms of the chromatographic separation order of the lanthanides. The results reported here can be used to manipulate separations parameters and column characteristics to better separate these lanthanide chelates. Fourteen chelates of the ligand 1,1,1-trifluoro-2,4-pentanedione are also thermally characterized but found to not sublime and be undesirable for this method. Additionally, all chelates are characterized by constant heating thermogravimetric analysis coupled with mass spectrometry, melting point analysis, elemental analysis and FTIR.
Funder
Office of Defense Programs Science and Technology Directorate
Publisher
Walter de Gruyter GmbH
Subject
Physical and Theoretical Chemistry
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