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Solubility and extraction of cerium(...

Andersen, Wendy Cook.

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Solubility and extraction of cerium(IV), terbium(III), and iron(III) beta-diketonates in supercritical carbon dioxide.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Solubility and extraction of cerium(IV), terbium(III), and iron(III) beta-diketonates in supercritical carbon dioxide./
Author:	Andersen, Wendy Cook.
Description:	139 p.
Notes:	Source: Dissertation Abstracts International, Volume: 61-07, Section: B, page: 3562.
Contained By:	Dissertation Abstracts International61-07B.
Subject:	Chemistry, Analytical. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=9979315
ISBN:	9780599853850

Solubility and extraction of cerium(IV), terbium(III), and iron(III) beta-diketonates in supercritical carbon dioxide.
Andersen, Wendy Cook.

Solubility and extraction of cerium(IV), terbium(III), and iron(III) beta-diketonates in supercritical carbon dioxide. - 139 p.

Source: Dissertation Abstracts International, Volume: 61-07, Section: B, page: 3562.

Thesis (Ph.D.)--University of Colorado at Boulder, 2000.

Supercritical fluid extraction with carbon dioxide and beta-diketone chelating agents is an attractive method for the separation of radioactive metal contaminants, such as plutonium, from aqueous solutions, contaminated soils and low-level radioactive waste. The inexpensive chelating agent 2,2,7-trimethyl-3,5-octanedione, H(tod), forms highly CO2-soluble chelates with the actinide surrogates, cerium(IV), iron(III) and terbium(III). NMR spectroscopy was used to estimate the acid dissociation, keto-enol equilibrium, and Fe(III) stability constants for H(tod) and the Fe(tod)3 complex, chemical properties that are important for designing extraction methods.

ISBN: 9780599853850Subjects--Topical Terms:

586156
Chemistry, Analytical.

Solubility and extraction of cerium(IV), terbium(III), and iron(III) beta-diketonates in supercritical carbon dioxide.
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100 1 $a Andersen, Wendy Cook. $3 1916084
245 1 0 $a Solubility and extraction of cerium(IV), terbium(III), and iron(III) beta-diketonates in supercritical carbon dioxide.
300 $a 139 p.
500 $a Source: Dissertation Abstracts International, Volume: 61-07, Section: B, page: 3562.
500 $a Director: Robert E. Sievers.
502 $a Thesis (Ph.D.)--University of Colorado at Boulder, 2000.
520 $a Supercritical fluid extraction with carbon dioxide and beta-diketone chelating agents is an attractive method for the separation of radioactive metal contaminants, such as plutonium, from aqueous solutions, contaminated soils and low-level radioactive waste. The inexpensive chelating agent 2,2,7-trimethyl-3,5-octanedione, H(tod), forms highly CO2-soluble chelates with the actinide surrogates, cerium(IV), iron(III) and terbium(III). NMR spectroscopy was used to estimate the acid dissociation, keto-enol equilibrium, and Fe(III) stability constants for H(tod) and the Fe(tod)3 complex, chemical properties that are important for designing extraction methods.
520 $a Ce(tod)4 and Tb2(tod)6 were synthesized and characterized by X-ray crystallography, elemental analysis, infrared spectroscopy, mass spectrometry, differential scanning calorimetry, and thermogravimetric analysis. The structure of Ce(tod)4 represents a new polymorph for tetrakis cerium chelates and Tb2(tod) 6 is the first reported dimeric beta-diketonate structure for terbium. These materials are promising precursor sources of cerium and terbium for thin film deposition, and are highly soluble in supercritical carbon dioxide, making them ideal surrogates for hazardous waste remediation using supercritical fluid extraction.
520 $a The solubilities of the cerium(IV), terbium(III), and iron(III) chelates of tod-, thd- (2,2,6,6-tetramethyl-3,5-octanedionate), and acac- (2,4-pentanedionate) were measured in supercritical carbon dioxide by near infrared spectroscopy from 40 to 60°C and 10 to 35 MPa with a high-pressure optical cell. Solubilities increased in the order acac < thd < tod for all metal beta-diketonates, with Ce(tod) 4, Tb(tod)3, and Fe(tod)3 an order of magnitude more soluble than Ce(thd)4, Tb(thd)3, and Fe(acac) 3, respectively. For the larger metal ions, Ce4+ and Tb3+, the flexibility of the isobutyl group in the tod ligand creates a more lipophilic shell around the central metal ion, increasing the solubility of the chelate in CO2. These observations indicate that the isobutyl group is at least as CO2-philic as the tert -butyl moiety. The experimental solubilities were correlated using the model proposed by Chrastil.
520 $a Finally, Ce4+, Tb3+, and Fe3+ were extracted from aqueous solutions and sand using H(tod) dissolved in supercritical CO2 to test the feasibility of this method. Extraction efficiencies of 38%, 76%, and 68% were obtained for Ce4+, Tb3+, and Fe3+ respectively. The effects of buffer, cosolvent, and auxiliary complexing agents were explored.
590 $a School code: 0051.
650 4 $a Chemistry, Analytical. $3 586156
650 4 $a Chemistry, Inorganic. $3 517253
650 4 $a Chemistry, Physical. $3 560527
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710 2 0 $a University of Colorado at Boulder. $3 1019435
773 0 $t Dissertation Abstracts International $g 61-07B.
790 1 0 $a Sievers, Robert E., $e advisor
790 $a 0051
791 $a Ph.D.
792 $a 2000
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=9979315