Journal of Nuclear and Radiochemical Sciences, Vol. 10, No. 2, pp. 7-12, 2009

Sequential Separation of U, Th, Pb, and Lanthanides with a Single Anion-Exchange Column
Yutaka Miyamoto,* Kenichiro Yasuda, Masaaki Magara, Takaumi Kimura, and Shigekazu
Usuda†
Research Group for Analytical Sciences, Nuclear Science and Engineering Directorate, JAEA Tokai-mura,Naka-gun, Ibaraki, 319-1195 Japan
Received: July 31, 2009; In Final Form: November 13, 2009
With a combination of a single anion-exchange column and mixed media of CH3COOH and other acids (HCl and/or HNO3), 50 ng each of U, Th, Pb, and the lanthanides were sequentially separated. The mixed media including
CH3COOH were effective for the sequential separation. All of the elements were more than 95% recovered, andthe decontamination factor was more than 100. Major elements in geological samples such as alkali metals, alkaline earth metals, and Fe were eliminated from the column. This separation technique reduces separation time andsimplifies the complicated traditional processes without any special reagents or equipments. The technique has
potential for use in pg (10 -12 g) level trace analysis.

19

1. Introduction
Uranium (U), thorium (Th), lead (Pb), and the lanthanides
are key elements in geochemistry and cosmochemistry.
Abundance ratios and isotopic ratios of these elements in rocks,
meteorites, and airborne dust are used for estimating their origin,1-3 dating of mineral formation,4 history of mineralization,58
and age determination of nuclear materials.9-11
Mass spectrometry is a powerful analytical method for thesestudies. Quantitative and isotopic analyses of these samples arecarried out with many types of mass spectrometers. Secondary
ion mass spectrometry (SIMS)12 and isotope microscopy13 provide isotopic analysis without any pre-treatments for µm-size
samples.4,5 They are the main analytical tools in geochemistry.
The total mass of some polyatomic ions, which are originatedin co-existing with other elements, sometimes overlap with thatof an isotope of interest and lead to systematic error in the measurement of isotopic ratios (e.g. 208 Pb12 C16 O + for 236 U and
195
Pt40Ar+ for 235U). Magara et al reported that the formation
rate of 195Pt40Ar+ measured by inductively-coupled plasma mass
spectrometry (ICP-MS) is 1.5 × 10 -5.14 The formation rate isdefined as the ratio of the count rate of 195Pt40Ar+ to 195Pt. Whenthe concentration ratio of Pt/U in an analytical sample is 10,
the atomic ratio of 235U/238U will include 0.7% of the systematic
error. The amount of Pt should be reduced to < 1/10 of the Uamount by means of a chemical separation to measure the isotopic ratios of U precisely. The contribution from the polyatomic ions may be subtracted if both the concentration ofinterfering elements and the formation rate can be measured
precisely. Esaka et al reported the technique of isolation of U
particles from Pb particles with a needle for analysis of U
minor isotopes by SIMS.15 The technique may be powerful forparticle analysis.
High concentrations of matrix elements, such as Na and K,
affect the ion intensity of analytes in ICP-MS measurements.16
Chemical separation of the elements of interest is classicallydone and is time-consuming, but precise analysis can only bedone by eliminating these interferences. Uranium, Th, Pb, andthe lanthanides can be separated with ion-exchange columns17*Corresponding author. E-mail: miyamoto.yutaka@jaea.go.jp
FAX: +81-29-284-3658†
Present address: Cyclotron and Radioisotope Center, Tohoku
University Aoba 6-3, Aramaki, Aoba-ku, Sendai, Miyagi, 980-8578
Japan

as well as with solvent extraction.20 Almost all these techniques require many complicated steps and various eluents. In
the precise analysis of µm-size samples, the chosen separation
procedures should be thought out to avoid contamination of theelements of interest from foreign environments. This type ofcontamination creates serious uncertainties in trace analyses.
Use of a clean laboratory and highly pure reagents are the mostimportant countermeasures for avoiding the contamination.
Many excellent ligands and extractants for the chemical separations are synthesized and available. 21-2 4 Many of thesereagents are often difficult to purify and they decompose,
whereas highly pure acids such as HCl, HNO3, CH3COOH, and
HF are readily available, and it is easy to purify them.
Hydrochloric acid and HNO3 are well known as eluents foranion-exchange separation. The ion-exchange characteristics ofall elements in these acids and mixture of some reagents suchas alcohols have been systematically studied since the 1960s.2530

To be effective at avoiding contamination from foreign environments, the separation procedure must be simplified. The
combination of multiple exchange columns for tasks such as
the evaporation of effluents increases the number of separation
steps, resulting in increase of a chance of contamination.
The authors developed a simplified separation technique forU, Th, Pb, and the lanthanides using a single anion-exchange
column and mixed media consisting of CH3COOH and otheracids. An anion-exchange column was used in this study.
Anion-exchange columns do not retain the elements of interest
from water and/or concentrated acids. It is therefore easy toclean anion-exchange columns. Cation-exchange columns
retain Th and the lanthanides over a wide range of HCl concentration (1–12 M). It is difficult to clean this type of column
completely.
There are few papers on the separation of these elementswith a single anion-exchange column. In this work, suitablecompositions of mixed media consisting of CH 3 COOH andother acids for the separations were investigated. Acetic acid isa good medium for an anion-exchange separation. It wasreported that the partial replacement of aqueous solution with
CH3COOH enhances the adsorption of many elements such asTh, U, Pb, and the lanthanides.31-35 Kim and Born reported thatthe distribution coefficients of U, Th, and Pa increase withincreasing concentration of CH 3 COOH and HCl in mixed
media of these acids.35 They explained that the hydration field© 2009 The Japan Society of Nuclear and Radiochemical Sciences
Published on Web 00/00/2009

MiyamotoJ. Nucl. Radiochem. Sci., Vol. 10, No. 2, 2009

around the uranium ion becomes weakened in the presence ofCH 3 COOH, and the water dipoles in coordination may bereplaced by acetate as well as chloride ions. The ion-exchange
characteristics of all the elements31-34 and the interaction ofactinides 36 were studied, but only a few applications with
CH3COOH media were reported.37-41
2. Experimental
Uranium, Th, Pb, and the lanthanides in a mixture of three
ICP-MS calibration solutions were separated with an anionexcha nge colum n and the m ixed media consisting of
CH3COOH and other acids. The elution profiles of these elements were examined, and the composition and volume of themixed media were optimized to achieve the sequential separation of the elements of interest. All the fractions of the effluent
were collected. The recovery of the elements in the fractions
was measured with an ICP-MS. The reagents and detailed procedures are described below.
2.1. Reagents. Three ICP-MS calibration solutions (XSTC13, XSTC-1, and XSTC-7, SPEX CertiPrep, Inc.) were mixed,
and a stock solution of 0.3 M HNO3 containing 103 ppb of U,
Th, Pb, lanthanides, etc. (57 elements) was prepared. The concentrations of these elements are shown in Table 1. Water wasdeionized and purified (resistivity: 18.2 MΩ·cm) with a MilliQ water system (Millipore Corp.). All labware such as vials
and stock bottles used in this study was made of Teflon (PFA).
The following commercially available reagents were used without further purification in this study.
HCl: concentration 30 wt.%, TAMA-Pure AA-100 grade,
TAMA Chemicals.
HNO3 : concentration 68 wt.%, TAMA-Pure AA-10 grade,
TAMA Chemicals.
HF: concentration 38 wt.%, TAMA-Pure AA-10 grade,
TAMA Chemicals.
CH3COOH: concentration >99.7wt.%, Extra pure grade fortrace analysis (UGR), Kanto Chemical Co. Ltd.
HI: concentration 55–58wt.%, Wako Pure Chemical
Industries, Ltd.
2.2. Ion Exchange Separation. About 550 mg (in dry
weight) of an anion-exchange resin (Muromac 1x8, Cl- form,
100–200 mesh, Muromachi Chemicals Inc.) was packed into apolyethylene column (5.5 mm i.d., 42 mm height, column volume: 1.0 mL). The column was washed with concentrated HCl
and H2O. Finally, the column was conditioned with 5 mL of the
mixture of CH3COOH and HNO3, which is the eluent for theelimination of alkali metals and alkaline earth metals. Stocksolution (500 µl) was pipetted into a 10 mL vial and evaporated
to dryness. About 50 ng of each element was contained in thesolution. The dried sample was dissolved in 1 mL of the mixture of CH3COOH and HNO3 and loaded onto the column. The
flow rate of the effluents was 0.1–0.2 mL/min for the mixed
media and 0.3–0.4 mL/min for the HCl media.
Each 4 mL of the effluent was collected into a separate vial.
The effluents were weighed and evaporated to dryness. The
resulting residues were dissolved in 1 mL of concentrated

HNO3, and the solutions were evaporated to dryness. Finally,
the residues were dissolved in 2 mL of 0.3 M HNO3 to analyze
the elemental concentration with an ICP-MS (Agilent 7500a,
Agilent Technologies Inc.). The stock solution was diluted, andsix standards of different concentrations were prepared to makea working curve. The variation of ion intensity among the samples in the ICP-MS measurement was corrected by bracketingthe measurement of samples with those of the standard solutions. The concentration of Fe was determined with the ion
intensity of mass 57, and the recovery of Fe from the column
was indicated as a relative value normalized to the total recovery of Fe in all effluent vials. All treatments were carried out
in clean rooms (ISO class 5 and 6) at the clean laboratory"CLEAR" in JAEA.42
3. Results and Discussion
The appropriateness of the eluent mixture, which consistedof mixture of CH3COOH and HCl and/or HNO3, was investigated by dividing the study into four parts, described in the following sections 3.1–3.4. Finally, the elements in interest weresequentially separated with the optimized eluents, and therecoveries were evaluated (see section 3.5.).
3.1. Elimination of alkali metals and alkaline earth metals. Alkali metals and alkaline earth metals such as Na, K,
Ca, and Mg are present in high concentrations in environmental samples such as rocks, soils, and plants. A high concentration of these elements may cause matrix effects in ICP-MS
analysis.16 By using mixed media consisting of CH3COOH and
HNO3 as the eluent, these elements were eliminated effectively.
The analytes—U, Th, Pb, and the lanthanides—were retained.
Figure 1 shows the effect of HNO3 concentration in themixed media on the elution of Lu. The mixture of 90 vol.%CH3COOH and 0.2 M HNO3 effectively suppressed the elutionof Lu. Lutetium (as a representative of the heavier lanthanides)
was eluted with more than 15 mL of the mixture. Lanthanum(as a representative of the lighter lanthanides), Th, Pb, and U
were retained after more than 30 mL of any mixture of
10
8
Lu recovery / %

8

0.6 M
0.5 M

6
4

0.4 M
0.1 M

2

0.2 M

0
0

5

10

15

20

25

30

35

Effluent volume / mL

Figure 1. Effect of HNO3 concentration in the mixed media of 90
vol.% CH3COOH and HNO3 on suppression of Lu elution. The column volume (CV) is equivalent to the effluent volume.

TABLE 1: Elemental concentration in the mixture of three ICP-MS calibration solutions
Concentration (ppb)Composition

Calibration solution

103(Li), Be, (Na), (Mg), (Al), (K), (Ca), V, Cr, Mn, Fe, Co, Ni, Cu, (Zn), Ga,
As, Se, Rb, Sr, Ag, Cd, In, Cs, Ba, (Hg), Tl, Bi, Pb, Th, U

XSTC-13 (10 µg/mL)

103
103

Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu
Ru, Rh, Pd, (Sn), Sb, Te, Hf, Ir, Pt, Au

XSTC-1 (10 µg/mL)
XSTC-7 (10 µg/mL)

Note: The calibration solutions were mixed and diluted with 0.3 M HNO3. The elements in parentheses were contained in the solution, but those were not determined in this work.

Sequential Separation of U, Th, Pb, and Lanthanides with a Single
40

Th recovery / %

30

20

10

0

0.5

0

1.0

1.5

2.0

Concentration of HNO3 / M

1.0

Cumulative recovery of La / %

100
La

0.8

80
Th
60

0.6

40

0.4

20

0.2

0

0

10

20
30
40
Effluent volume / mL

50

Cumulative recovery of Th / %Figure 2. Effect of HNO3 concentration in the mixed media of
CH3COOH, HCl, and HNO3 on suppression of Th elution. The recovery of Th in 9 mL of effluent is indicated. The concentrations of
CH 3COOH and HCl were 78–90 vol.% and 0.76–0.95 M, respectively.

0

Figure 3. Cumulative recovery of La and Th eluted with the mixed
media of 85.0 vol.% CH3COOH + 0.89 M HCl + 0.80 M HNO3. The
column volume (CV) is equivalent to the effluent volume.

104
102
Recovery / %CH3COOH and HNO3. Thirteen mL (13 column volumes, CV)of the mixture was used for the elimination of alkali metals
and alkaline earth metals from the column.
The heavier lanthanides—Lu, Yb, Tm, Er, Ho, Dy, Tb, andGd—were eluted with more than 15 mL of the mixture in thatorder (i.e. the inverse order of their atomic number). Thisimplies that the distribution coefficients (Kd) of the heavier lanthanides decreased in the order of their atomic number.
Korkisch reported the Kd of U, Th, Pb, La, and Gd on Dowex
1x8 with a mixed media consisting of glacial CH3COOH and
HNO3.43 The Kd of these elements increase with increasing concentration of CH 3 COOH, and these elements are strongly
retained by the resin from a mixture of 90 vol.% CH3COOH
and 10 vol.% 5 M HNO3. He also reported that the Kd of La
slightly increases with increasing acidity, and the Kd of Gd is
one tenth that of La. The trend on the elution profiles of lanthanides in this work was consistent with his results and theexperimental results on the anion-exchange separation with
HNO3 media.44-47
3.2. Separation of lanthanides. It is known that U and Pb
are retained by anion-exchange columns in HCl media, and Th
and the lighter lanthanides (La) are retained in HNO3 media.48
We found that a mixed media solution consisting of CH3COOH,
HCl, and HNO3 was a good eluent for the separation of lanthanides from U, Th, and Pb.
Figure 2 shows the effect of HNO3 concentration on therecovery of Th. The concentrations of CH 3 COOH and HCl
were 78–90 vol.% and 0.76–0.95 M, respectively. The recoveries of Th in 9 mL of the effluent decreased with increasing
HNO3 concentration in the mixed media. Thorium was noteluted when the HNO3 concentration was more than 0.5 M. The
mixture of 85.0 vol.% CH 3COOH, 0.89 M HCl, and 0.80 M
HNO3 was the best composition for separation of the lanthanides. Figure 3 shows the cumulative recoveries of La andTh. The recovery of La reached 100% with 35 mL of this mixture, and Th was eluted with more than 35 mL. Therefore, lanthanides were separated from Th, Pb, and U with 37 mL (37CV) of this eluent.
The recovery of Ce was irregularly low (35%) comparedwith that of the other lanthanides (95%). To improve the recovery of Ce, some reducing agents (NH 2 OH·HCl, HI, H 2 O 2 ,NH4NO2) were added to the eluents, and Ce4+ was changed into
Ce3+. Hydroxylamine chloride (NH 2 OH·HCl) was the mosteffective of these four reagents for improving the recovery of
Ce. Cerium recovery increased with the reducing agents in thefollowing order: NH 2OH·HCl > HI > H 2O2 > NH4NO2 . Thisorder is the same as that of their standard electrode potential,
and may depend on the strength of reduction of Ce 4+ to Ce3+.
Cerium in the ICP-MS solution was prepared from Ce(NO3)3.
The valence of Ce in the initial feed solution may be mainly
trivalent, and it is the same as that of other lanthanides. Someof Ce3+ ions might be oxidized to Ce 4+ during the chemicaltreatments, and this oxidation may cause the anomalously low
recovery of Ce.
By using the mixture of 85.0 vol.% CH3COOH, 0.89 M HCl,
0.80 M HNO3, and 0.01 M NH2OH·HCl, all of the lanthanides
were fully recovered (99.7 ± 0.7%) as shown in Figure 4. There
was no difference in recovery among the lanthanides. It is possible to determine each lanthanide in a sample without individual recovery correction.
3.3. Separation of Th from Pb and U. Thorium was separated with the mixture of CH3COOH and HCl. The elution profile of Th was affected by the concentrations of both HCl andCH 3 COOH. The elution shape of Th became sharper withdecreasing CH3COOH concentration, as shown in Figure 5(a).
The elution position of Th was shifted to the front with increasing HCl concentration, as shown in Figure 5(b). It seems to bepreferable to use the mixture of 60 vol.% CH3COOH and 1 M
HCl for the Th separation, but 2–4% of the Pb was eluted

9

J. Nucl. Radiochem. Sci., Vol. 10, No. 2, 2009

100
98
96
94
La Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu

Figure 4. Variation in the recovery of lanthanides eluted with themixed media of 85.0 vol.% CH3COOH + 0.89 M HCl + 0.80 M HNO3
+ 0.01 M NH2OH·HCl. The solid line and the broken lines show theaverage and standard deviation (1σ) of recovery of lanthanides,
respectively; (99.7 ± 0.7) %.

together with the Th for this composition. We found that 22 mLof the mixture of 70 vol.% CH3COOH and 1 M HCl worked
well for the Th separation in this work. Lead was not eluted
with this eluent mixture.
To improve the elution shape of Th, 0.005 M HF was added
to the eluent. The shape became sharp, and 99% of Th was

10Miyamoto

J. Nucl. Radiochem. Sci., Vol. 10, No. 2, 2009

eluted with 10 mL of the eluent. The formation of cationic fluoro complexes of Th may reduce the absorbability of Th in ananion-exchange column.
3.4. Separation of Pb, U, and Fe. Lead, Fe, and U wereseparated with the conventional eluents. Thirteen mL of 9 M
HCl, 24 mL of 9 M HCl + 0.1 M HI, and 25 mL of 0.5 M HCl+ 0.005 M HF were used for Pb separation, Fe elimination, andU separation, respectively. Iron was eliminated from the column by reducing Fe3+ to Fe2+ with 9 M HCl + 0.1 M HI. The
column stood for 10 hours after eluting with 2 mL of the eluent
to ensure the reduction, then Fe was eliminated with 22 mL ofthe eluents. The elution shape of U was sharpened with a mix-

100

Th recovery / %

80

60

40

80%
70%
60%

20

0

0

5

10

15

20

25

Effluent volume / mL

Figure 5(a). Effect of the concentration of CH3COOH in the mixed
media of CH3COOH (60 vol.%, 70 vol.%, and 80 vol.%) and 1 M HClon the elution profile of Th. The elution curves indicate the results ofthe fits by the Glueckauf equation.49 The column volume (CV) is
equivalent to the effluent volume.

ture of HCl and HF. This probably occurs for the same reason
as the Th elution. Schumann et al. reported that UO2 2+ andUO2F+ are the main cation species of U in a mixture of 0.001–
0.1 M HF and 0.1 M HCl.50
3.5. Sequential separation with the optimized eluents. By
using the eluents optimized in sections 3.1. to 3.4., sequential
separation of the elements of interest was carried out. Figure 6
shows elution curves of the elements of interest and representative interfering and matrix elements. Table 2 shows the eluted
elements whose recovery was more than 20% in the fractions.
The recovery of U, Th, Pb, and the lanthanides in each fraction(fraction No.6, fraction No.3, fraction No.4, and fraction No.2
in Figure 6) were 82%, 97%, 100%, and 100%, respectively.
The recovery of U was more than 95% without the Fe separation using HCl + HI. This variation of U recovery might becaused by iodine adsorption on a portion of the surface of theresin, which is an oxidized product of HI. The recovery of Pb
was estimated as 100% in this sequential separation, but 500
pg of Pb was contained in all of the fractions as a process
blank, especially 2 ng (equivalent to 4% of total Pb) in the fraction No.5. The excess Pb may originate from the labware, thereagents such as HI and very fine (< 0.3 µm in diameter) Pb
aerosols which are passed through the HEPA filters built in theclean rooms and clean hoods. A portion of Fe was eluted in theTh fraction (fraction No.3 in Figure 6) (14%) and the U fraction (fraction No.6 in Figure 6) (10%). Decontamination factors(DF) are shown in Table 3. The DF of lanthanides to Th, Th toPb, and Pb to U were more than 100. Less than 1% of the alkali
metals and 4% of the alkaline earth metals were contained in
the lanthanides fraction (fraction No. 2 in Figure 6). We foundthat each element of interest was satisfactorily separated andfully recovered by this technique.
4. Conclusion
With a single anion-exchange column, sequential separationof 50 ng each of U, Th, Pb, and the lanthanides in an ICP-MS
calibration solution was successfully carried out. Using a mixture of CH3COOH and other mineral acids (HCl and/or HNO3)

1

100
Recovery / %

100
0.5M

80

2

Th

3

Pb 4

U

80
Lu

stand for
10 h

40

(Pb)

0
100 Rb

1M
0.2M

Recovery / %Th recovery / %6Interests

La

60

20

60

5

40

Interferences

Sr

80
60

Y
Fe

40

stand for
10 h

Sc

20
0

20

(Fe)

0

20

40

60

(Fe)

80

100

120

Effluent volume / mL

0

0

5

10

15

20

25

Effluent volume / mL

Figure 5(b). Effect of the concentration of HCl in the mixed mediaof HCl (0.2 M, 0.5 M, and 1.0 M) and 80 vol.% CH 3COOH on theelution profile of Th. The elution curves indicate the results of the fits
by the Glueckauf equation.49 The column volume (CV) is equivalent
to the effluent volume.

Figure 6. Sequential elution curves of U, Th, Pb, and the lanthanides(La and Lu) (upper), and elution curves of some interfering elements,
Rb (representative of alkaline metals), Sr (representative of alkaline
earth metals), Sc, Y, and Fe (bottom). Eluents; No.1: 90 vol.%CH3COOH + 0.2 M HNO3 (13 mL); No.2: 85.0 vol.% CH3COOH +0.89 M HCl + 0.80 M HNO3 + 0.01 M NH2OH·HCl (37 mL); No.3:
70 vol.% CH3COOH + 1 M HCl + 0.005 M HF (22 mL); No.4: 9 M
HCl (13 mL); No.5: 9 M HCl + 0.1 M HI (2 mL and stand for 10hours, then 22 mL); No.6: 0.5 M HCl + 0.005 M HF (25 mL). The
column volume (CV) is equivalent to the effluent volume.

Sequential Separation of U, Th, Pb, and Lanthanides with a Single

J. Nucl. Radiochem. Sci., Vol. 10, No. 2, 200911

TABLE 2: Eluted elements in each fraction
Fraction No.
1
2

Eluents

Eluted elements
Be, Sc, (V), Cr, Mn, Ni. (As), Se, Rb, Sr, (Ru),Te, Cs, Ba, (Tl)

90 vol.% CH3COOH + 0.2 M HNO3 (13 mL)
85.0 vol.% CH3COOH + 0.89 M HCl + 0.80 M HNO3 +0.01 M NH2OH·HCl (37 mL)
70 vol.% CH3COOH + 1 M HCl + 0.005 M HF (22 mL)
9 M HCl (13 mL)
9 M HCl + 0.1 M HI (24 mL)
0.5 M HCl + 0.005 M HF (25 mL)

Sc, V, Cr, Mn, Ni, Se, Y, (Ba), lanthanides, (Ir)Mn, Co, Th
Co, Cu, (Rh), In, Pb
Fe
Ga, As, U
Note: The elements whose recovery was more than 20% of the fraction are tabulated. The elements whose recovery was in therange of 15–20% are shown in parentheses. The elements expected to be eluted in the fraction are indicated in bold type.
3
4
5
6

TABLE 3: Decontamination factors of representative elements in the effluents
Fraction No.2

Fraction No.3

Fraction No.6

La / Th > 540
La / Rb 130
La / Sr
22
La / Sc
1.8
La / Y
1.0

Th / La 720
Th / Pb > 110
Th / Fe
7

U / Pt > 130
U / Pb > 140
U / Fe10Note: The decontamination factor is calculated from therecovery ratio of the element of interest to the co-existing element in the fraction.
enabled complete separation of the elements of interest. The
absorption of the elements of interest on the column wasenhanced in the mixture of CH3COOH compared with simple
HCl and HNO3 media. Alkali metals, alkaline earth metals,
and Fe which are representative interferences for isotopic analysis in geological samples were eliminated from U, Th, Pb, andthe lanthanides. The recovery of the elements of interest wasmore than 95%. The elution shapes of Th and U became sharp
by adding 0.005 M HF to the eluents. The recovery of Ce
increased by adding 0.01 M NH 2OH·HCl to the eluent for thelanthanide separation, and all of the lanthanides, including Ce,
were fully recovered. Due to the tailing of the Fe elution, 10%of the Fe was eluted in the U fraction. The separation performance (e.g., peak resolution) may be improved by controllingthe column size and the grain size of the resin. This simplified
separation technique can be applied for pg (10 -12 g) level trace
analysis with highly pure reagents. This separation technique
has potential of applications in many research and development
field, such as geochemistry, cosmochemistry, and analysis for
non-proliferation.
References(1) A. Bollhöfer and K. J. R. Rosman, Geochim. Cosmochim.
Acta 65, 1727 (2001).
(2) A. Bollhöfer and K. J. R. Rosman, Geochim. Cosmochim.
Acta 64, 3251 (2000).
(3) S. Richter, A. Alonso, W. De Bolle, R. Wellum, and P. D. P.
Taylor, Int. J. Mass Spectrom. 193, 9 (1999).
(4) I. G. Alvarez, M. A. Kusiak, and R. Kerrich, Chem. Geol.
230, 140 (2006).
(5) E. Pelt, F. Chabaux, C. Innocent, A. K. Navarre-Sitchler, P.
B. Sak, and S. L. Brantley, Earth Planet. Sci. Lett. 276, 98(2008).
(6) R. A. Mortlock, R. G. Fairbanks, T. -C. Chiu, and J.
Rubenstone, Geochim. Cosmochim. Acta 69, 649 (2005).
(7) K. Horie and H. Hidaka, Radiochim. Acta 92, 805 (2004).
(8) H. Bem and F. Bou-Rabee, Environ. Int. 30, 123 (2004).

(9) H. T. Zhang, F. R. Zhu, J. Xu, Y. H. Dai, D. M. Li, X. W.
Yi, L. X. Zhang, and Y. G. Zhao, Radiochim. Acta 96, 327(2008).
(10) M. Wallenius, A. Morgenstern, C. Apostolidis, and K.
Mayer, Anal. Bioanal. Chem. 374, 379 (2002).
(11) M. Wallenius and K. Mayer, Fresnius J. Anal. Chem. 366,
234 (2000).
(12) Y. L. Chen, D. P. Li, J. Zhou, F. Liu, H. F. Zhang, L. S.
Nie, L. T. Jiang, B. Song, X. M. Liu, and Z. Wang,
Geochem. J. 43, 77 (2009).
(13) K. Nagashima and H. Yurimoto, Geochim. Cosmochim.
Acta 70, A440 (2006).
(14) M. Magara, T. Sakakibara, S. Kurosawa, M. Takahashi, S.
Sakurai, Y. Hanzawa, F. Esaka, K. Watanabe, and S. Usuda,
J. Nucl. Sci. Technol. 39, 308 (2002).
(15) F. Esaka, K. T. Esaka, C. G. Lee, M. Magara, S. Sakurai, S.
Usuda, and K. Watanabe, Taranta 71, 1011 (2007).
(16) M. Magara, T. Sakakibara, S. Kurosawa, M. Takahashi, S.
Sakurai, Y. Hanzawa, F. Esaka, K. Watanabe, and S. Usuda,
J. Aanl. At. Spectrom. 17, 1157 (2002).
(17) G. Shimoda, J. Mass Spectrom. Soc. Jpn. 52, 213 (2004).
(18) E. H. Borai and A. S. Mady, Appl. Radiat. Isot. 57, 463(2002).
(19) F. Tera and G. J. Wasserburg, Anal. Chem. 47, 2214
(1975).
(20) T. Yokoyama, A. Makishima, and E. Nakamura, Anal.
Chem. 71, 135 (1999).
(21) E. Metwally, A. Sh. Saleh, and H. A. El-Naggar, J. Nucl.
Radiochem. Sci. 6, 119 (2005).
(22) B. Gupta, P. Mlik, and A. Deep, J. Radioanal. Nucl. Chem.
251, 451 (2002).
(23) E. P. Horwiz, M. L. Dietz, S. Rhoads, C. Felinto, N. H.
Gale, and J. Houghton, Anal. Chim. Acta 292, 263 (1994).
(24) E. P. Horwiz, M. L. Dietz, R. Chiarizia, and H. Diamond,
Anal. Chim. Acta 266, 25 (1992).
(25) S. Usuda, J. Radioanal. Nucl. Chem. 123, 619 (1988).
(26) S. F. Marsh, J. E. Alarid, C. F. Hammond, M. J. McLead,
F. R. Roensch, and J. E. Rein, Los Alamos ScientificLaboratory Report, LA-7084 (1978).
(27) J. P. Faris and R. F. Buchanan, Anal. Chem. 36, 1157
(1964).
(28) J. Korkisch and G. E. Janauer, Talanta 9, 957 (1962).
(29) J. P. Faris, Anal. Chem. 32, 520 (1960).
(30) F. Nelson, R. M. Rush, and K. A. Kraus, J. Am. Chem.
Soc. 82, 339 (1960).
(31) P. Van Acker, Anal. Chim. Acta 113, 149 (1980).
(32) P. Van den Winkel, F. De Corte, and J. Hoste, J. Radioanal.
Chem. 10, 139 (1972).
(33) P. Van den Winkel, F. De Corte, and J. Hoste, Anal. Chim.
Acta 56, 241 (1971).
(34) P. Van den Winkel, F. De Corte, A. Speecke, and J. Hoste,
Anal. Chim. Acta 42, 340 (1968).

12

J. Nucl. Radiochem. Sci., Vol. 10, No. 2, 2009(35) J. I. Kim and H. -J. Born, Radiochim. Acta 14, 65 (1970).
(36) L. Rao, P-L. Zanonato, and P. D. Bernardo, J. Nucl.
Radiochem. Sci. 6, 31 (2005).
(37) L. I. Guseva, G. S. Tikhomirova, and P. A. Korovaikov,
Radiochemisty (Radiokhimiya) 41, 229 (1999).
(38) G. S. Tikhomirova, L. I. Guseva, and P. A. Korovaikov,
Radiochemisty (Radiokhimiya) 41, 233 (1999).
(39) E. Toda, A. Hioki, and M. Kubota, Anal. Chim. Acta 333,
51 (1996).
(40) M. O. Petropulu and P. Schramel, Anal. Chim. Acta 313,
243 (1995).
(41) S. V. Kulkarni, S. K. Soman, and S. S. Joshi, J. Indian
Chem. Soc. 60, 779 (1983).
(42) S. Usuda, K. Yasuda, Y. S. Kokubu, F. Esaka, C. -G. Lee,
M. Magara, S. Sakurai, K. Watanabe, F. Hirayama, H.

Miyamoto
Fukuyama, K. T. Esaka, K. Iguchi, Y. Miyamoto, and J. -Y.
Chai, Intern. J. Environ. Anal. Chem. 86, 663 (2006).
(43) J. Korkisch, Anal. Chem. 36, 850 (1964).
(44) S. K. Sungur and A. Akseli, J. Chromatogr. A 874, 311(2000).
(45) S. Usuda, J. Radioanal. Nucl. Chem. 111, 399 (1987).
(46) S. Usuda and M. Magara, J. Radioanal. Nucl. Chem. Lett.
119, 67 (1987).
(47) Y. Marcus and F. Nelson, J. Phys. Chem. 63, 77 (1959).
(48) K. A. Kraus and F. Nelson, Am. Soc. for Testing Materials,
Special Technical Publication, 195, 27 (1956).
(49) E. Glueckauf, Trans. Faraday Soc. 51, 34 (1955).
(50) D. Schumann, M. Andrassy, H. Nitsche, A. F. Novgorodov,
and H. Bruchertseifer, Radiochim. Acta 79, 217 (1997).