Abstract
Results of an inter-laboratory round-robin study of the application of time-resolved emission spectroscopy (TRES) to the speciation of uranium(VI) in aqueous media are presented. The round-robin study involved 13 independent laboratories, using various instrumentation and data analysis methods. Samples were prepared based on appropriate speciation diagrams and, in general, were found to be chemically stable for at least six months. Four different types of aqueous uranyl solutions were studied: (1) acidic medium where UO22+aq is the single emitting species, (2) uranyl in the presence of fluoride ions, (3) uranyl in the presence of sulfate ions, and (4) uranyl in aqueous solutions at different pH, promoting the formation of hydrolyzed species. Results between the laboratories are compared in terms of the number of decay components, luminescence lifetimes, and spectral band positions. The successes and limitations of TRES in uranyl analysis and speciation in aqueous solutions are discussed.
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References
1.
Billard
I.
Lützenkirchen
K.
, Radiochim. Acta, paper accepted (2002 ).
2.
Geipel
G.
Brachmann
A.
Brendler
V.
Bernhard
G.
Nitsche
H.
, Radiochim. Acta 75 , 199 (1996 ).
3.
Aas
W.
Steinle
E.
Fanghänel
T.
Kim
J. I.
, Radiochim. Acta 84 , 85 (1999 ).
4.
Arisaka
M.
Kimura
T.
Suganuma
H.
Yoshida
Z.
, Radiochim. Acta 90 , 193 (2002 ).
5.
Moulin
C.
Decambox
P.
Mauchien
P.
, J. Radioanal. Nucl. Chem. 226 , 135 (1997 ).
6.
Kato
Y.
Meinrath
G.
Kimura
T.
Zenko
Y.
, Radiochim. Acta 64 , 107 (1994 ).
7.
Berthoud
T.
Decambox
P.
Kirsch
B.
Mauchien
P.
Moulin
C.
, Anal. Chem. 60 , 1296 (1988 ).
8.
Scapolan
S.
Ansoborlo
E.
Moulin
C.
Madic
C.
, J. Alloys Compd. 271/273 , 106 (1998 ).
9.
Fujimori
H.
Matsui
T.
Suzuki
K.
, J. Nucl. Sci. Technol. 25 , 798 (1988 ).
10.
Lopez
M.
Birch
D. J. S.
, Chem. Phys. Lett. 268 , 125 (1997 ).
11.
Couston
L.
Pouyat
D.
Moulin
C.
Decambox
P.
, Appl. Spectrosc. 49 , 349 (1995 ).
12.
Yamamura
T.
Park
Y. Y.
Tomiyasu
H.
, J. Alloys Compd. 193 , 186 (1993 ).
13.
Kitamura
A.
Yamamura
T.
Hase
H.
Yamamoto
T.
Moriyama
H.
, Radiochim. Acta 82 , 147 (1998 ).
14.
Leung
A.
Hayashibara
L.
Spadaro
J.
, J. Phys. Chem. Solids 60 , 299 (1999 ).
15.
Rutsch
M.
Geipel
G.
Brendler
V.
Bernhard
G.
Nitsche
H.
, Radiochim. Acta 86 , 135 (1999 ).
16.
Eliet
V.
Grenthe
I.
Bidoglio
G.
, Appl. Spectrosc. 54 , 99 (2000 ).
17.
Addleman
R. S.
Wai
C. M.
, Anal. Chem. 72 , 2109 (2000 ).
18.
Gabriel
U.
Charlet
L.
Schlâper
C. W.
Vial
J. C.
Brachmann
A.
Geipel
G.
, J. Colloid Interface Sci. 239 , 358 (2001 ).
19.
Jorgensen
C.
Reisfeld
R.
, J. Electrochem. Soc. 130 , 683 (1983 ).
20.
Baird
C. P.
Kemp
T. J.
, Prog. React. Kinet. 22 , 87 (1997 ).
21.
Marcantonatos
M. D.
, Inorg. Chim. Acta 24 , 37 (1977 ).
22.
Formosinho
S. J.
Miguel
M. G.
Burrows
H. D.
, J. Chem. Soc., Faraday Trans 1 80 , 1717 (1984 ).
23.
Burrows
H. D.
Cardoso
A. C.
Formosinho
S. J.
Gil
A. M. P. C.
Miguel
M. G.
, J. Photochem. Photobiol., A 68 , 279 (1992 ).
24.
Denning
R. G.
, Struct. Bonding (Berlin) 79 , 215 (1992 ).
25.
Görller-Walrand
C.
De Jaegere
S.
, Spectrochim. Acta, Part A 28 , 257 (1972 ).
26.
Meinrath
G.
Klenze
R.
Kim
J. I.
, Radiochim. Acta 74 , 81 (1996 ).
27.
Jensen
M. P.
Choppin
G. R.
, Radiochim. Acta 82 , 83 (1998 ).
28.
Moulin
C.
Beaucaire
C.
Decambox
P.
Mauchien
P.
, Anal. Chim. Acta 238 , 291 (1990 ).
29.
Moulin
C.
Laszak
I.
Moulin
V.
Tondre
C.
, Appl. Spectrosc. 52 , 528 (1998 ).
30.
Duff
M. C.
Morris
D. E.
Hunter
D. B.
Bertsch
P. M.
, Geochim. Cosmochim. Acta 64 , 1535 (2000 ).
31.
Bernhard
G.
Geipel
G.
Brendler
V.
Nitsche
H.
, Radiochim. Acta 74 , 87 (1996 ).
32.
Van der Lee
J.
, Thermodynamics and Mathematical Concepts of CHESS (CIG-Ecole des Mines de Paris , Fontainebleau , 1998 ).
33.
Grenthe
I.
, Chemical Thermodynamics of Uranium (H. Wanner and I. Forest , Amsterdam , 1992 ).
34.
Meinrath
G.
Hurst
S.
Gatzweiller
R.
, Fresenius' J. Anal. Chem. 368 , 561 (2000 ).
35.
Sémon
L.
Boehme
C.
Billard
I.
Hennig
C.
Lützenkirchen
K.
Reich
T.
Rossberg
A.
Rossini
I.
Wipff
G.
, Chem. Phys. Chem. 2 , 101 (2001 ).
36.
Mesley
R. J.
Pocklington
W. D.
Walker
R. F.
, Analyst (Cambridge, U.K.) 116 , 975 (1991 ).
37.
Bouby
M.
Billard
I.
Bonnenfant
A.
Klein
G.
, Chem. Phys. 240 , 353 (1999 ).
38.
Meinrath
G.
Kato
Y.
Yoshida
Z.
, J. Radioanal. Nucl. Chem. 174 , 299 (1993 ).
39.
Azenha
M. E.
Burrows
H. D.
Formosinho
S. J.
Miguel
M. G.
Daramagnyan
A. P.
Khudiakov
I. V.
, J. Lumin. 48/49 , 522 (1991 ).
40.
Horrocks
W. d. J.
Sudnick
D. R.
, J. Am. Chem. Soc. 101 , 334 (1979 ).
41.
Beitz
J. V.
Williams
C.
, J. Alloys Compd. 250 , 375 (1997 ).
42.
Moriyasu
M.
Yokoyama
Y.
Ideka
S.
, J. Inorg. Nucl. Chem. 39 , 2199 (1977 ).
43.
Fazekas
Z.
Yamamura
T.
Tomiyasu
H.
, J. Alloys Compd. 271/273 , 756 (1998 ).
44.
Moulin
C.
Decambox
P.
Trecani
L.
, Anal. Chim. Acta 321 , 121 (1996 ).
45.
Billard
I.
Rustenholtz
A.
Sémon
L.
Lützenkirchen
K.
, Chem. Phys. 270 , 345 (2001 ).
46.
Moulin
C.
Decambox
P.
Moulin
V.
Decaillon
J. G.
, Anal. Chem. 67 , 348 (1995 ).
47.
Park
Y. Y.
Sakai
Y.
Abe
R.
Ishii
T.
Harada
M.
Kojima
T.
Tomiyasu
H.
, J. Chem. Soc., Faraday Trans. 86 , 55 (1990 ).
48.
Meinrath
G.
Lis
S.
Stryla
Z.
Noubactep
C.
, J. Alloys Compd. 300/301 , 107 (2000 ).
49.
Moll
H.
Geipel
G.
Brendler
V.
Bernhard
G.
Nitsche
H.
, J. Alloys Compd. 271/273 , 765 (1998 ).
50.
Beechem
J. M.
Ameloot
M.
Brand
L.
, Chem. Phys. Lett. 120 , 466 (1985 ).
51.
Janssens
L. D.
Boens
N.
Ameloot
M.
De Schryver
F. C.
, J. Phys. Chem. 94 , 3564 (1990 ).
52.
Adams
M. J.
, Chemometrics in Analytical Spectroscopy (N. W. Barnett , Cambridge , 1995 ).
53.
Czerwinski
K. R.
Buckau
G.
Scherbaum
F.
Kim
J. I.
, Radiochim. Acta 65 , 111 (1994 ).