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Title: f-state luminescence of lanthanide and actinide ions in solution

Abstract

Detailed studies of the luminescence of aquated Am{sup 3+} are presented in the context of prior lanthanide and actinide ion work. The luminescing state of aquated Am{sup 3+} is confirmed to be {sup 5}D{sub l} based on observed emission and excitation spectra. The luminescence lifetime of Am{sup 3+} in H{sub 2}O solution is (22 {plus_minus} 3) ns and (155 {plus_minus} 4) ns in D{sub 2}O solution at 295 K. Judd-Ofelt transition intensity theory qualitatively describes the observed Am{sup 3+} relative integrated fluorescence intensities. Recent luminescence studies on complexed trivalent f-element ions in solution are reviewed as to the similarities and differences between lanthanide ion 4f state and actinide ion 5f state properties.

Authors:
Publication Date:
Research Org.:
Argonne National Lab., IL (United States)
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10180770
Report Number(s):
ANL/CHM/CP-79390; CONF-9309142-2
ON: DE93019756; TRN: 93:020062
DOE Contract Number:
W-31109-ENG-38
Resource Type:
Conference
Resource Relation:
Conference: 20. rare earth research conference,Monterey, CA (United States),12-17 Sep 1993; Other Information: PBD: [1993]
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; AMERICIUM IONS; LUMINESCENCE; FLUORESCENCE; AQUEOUS SOLUTIONS; LIFETIME; HEAVY WATER; PERCHLORIC ACID; F STATES; EMISSION SPECTRA; 400702; 400500; PROPERTIES OF RADIOACTIVE MATERIALS; PHOTOCHEMISTRY

Citation Formats

Beitz, J.V. f-state luminescence of lanthanide and actinide ions in solution. United States: N. p., 1993. Web.
Beitz, J.V. f-state luminescence of lanthanide and actinide ions in solution. United States.
Beitz, J.V. 1993. "f-state luminescence of lanthanide and actinide ions in solution". United States. doi:. https://www.osti.gov/servlets/purl/10180770.
@article{osti_10180770,
title = {f-state luminescence of lanthanide and actinide ions in solution},
author = {Beitz, J.V.},
abstractNote = {Detailed studies of the luminescence of aquated Am{sup 3+} are presented in the context of prior lanthanide and actinide ion work. The luminescing state of aquated Am{sup 3+} is confirmed to be {sup 5}D{sub l} based on observed emission and excitation spectra. The luminescence lifetime of Am{sup 3+} in H{sub 2}O solution is (22 {plus_minus} 3) ns and (155 {plus_minus} 4) ns in D{sub 2}O solution at 295 K. Judd-Ofelt transition intensity theory qualitatively describes the observed Am{sup 3+} relative integrated fluorescence intensities. Recent luminescence studies on complexed trivalent f-element ions in solution are reviewed as to the similarities and differences between lanthanide ion 4f state and actinide ion 5f state properties.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = 1993,
month = 9
}

Conference:
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  • The possibility of separating the trivalent lanthanides, represented by EU{sup 3+}, and actinides, represented by Cf{sup 3+}, using HDEHP in toluene and an aqueous phase containing N-piperidinomethane-1,1-diphosphotic acid, PMDPA, has been investigated. This modified aqueous phase offers potential advantages over the diethylenetriaminepentaacetic acid based TALSPEAK process because of the improved complexation properties of PMDPA in acidic solutions, and the ability to decompose PMDPA before disposal. Extraction experiments were conducted at 25 C in 2 M NaClO{sub 4} between -log [H{sup +}] 1 and 2. The studies enabled us to derive the aqueous phase speciation, the stability constants of the aqueousmore » complexes, and the Cf/Eu separation factors. Despite the presence of an amino group in PMDPA that should favor the retention of the actinides in the aqueous phase, the Cf/Eu separation factors are near unity under the conditions studied.« less
  • The neutron scattering difference method is described and applied to investigations of the aqua rare-earth ions, Nd/sup 3 +/ and Dy/sup 3 +/. Metal-water distances and hydration numbers have been unambiguously determined for these ions' inner coordination spheres. The values of the hydration number, n, of 8.5 +- 0.2 for Nd/sup 3 +/ and 7.4 +- 0.5 for Dy/sup 3 +/, directly support the claim of Spedding et al. that n decreases by one unit across the lanthanide series. The possible application of this method to actinide ions in solution is also discussed. 7 refs., 4 figs.
  • This paper reviews some of the recent developments in this area of spectroscopy, emphasizing the optical properties of the tripositive lanthanide and actinide ions. In particular, the single ion properties of line positon, intensity, width, and fluorescence lifetime are discussed. 53 reference, 3 figures, 4 tables.
  • The thermodynamic data for complexation of trivalent lanthanide and actinide cations with halate and haloacetate anions are reported. These data are analyzed for estimates of the relative amounts of inner (contact) and outer (solvent separated) sphere complexation. The halate data reflected increasing inner sphere character as the halic acid pK/sub a/ increased. Use of a Born-type equation with the haloacetic acid pK/sub a/ values allowed estimation of the effective charge of the carboxylate group. These values were, in turn, used to calculate the inner sphere stability constants with the M(III) ions. This analysis indicates increasing the inner sphere complexation withmore » increasing pK/sub a/ but relatively constant outer sphere complexation.« less
  • The applicability of the EXAFS technique in the study of actinide systems is discussed. Uranium L/sub III/-edge spectra obtained on an in-lab rotating anode EXAFS facility are presented and analyzed for crystalline UO/sub 2/F/sub 2/ and aqueous solutions containing hexavalent uranium ions. Methods for the extension of the technique to more dilute systems are discussed.