VAEC-AR 06--33

STUDY ON ANALYTICAL METHODS OF TELLURIUM

CONTENT IN NATRIIODIDE (Na131I) RADIOPHARMACEUTICAL
SOLUTION PRODUCED IN THE DALAT NUCLEAR REACTOR
Vo Thi Cam Hoa, Duong Van Dong, Nguyen Thi Thu, Chu Van Khoa,
Bui Van Cuong, Mai Phuoc Tho, Pham Ngoc Dien and Nguyen Thanh Binh
Nuclear Research Institute
Abstract: This annual report describes the practical methods for analyzing of
Tellurium content in Na131I solution produced at the Dalat Nuclear Research Institute.
We studied analytical methods to control Tellurium content in final Na131I solution
product used in medical purposes by three methods such as: spot test, gamma
spectrometric and spectrophotometeric methods.
These investigation results are shown that the spot test method is suitable for controlling
Tellurium trace in the final product. This spot test can be determinate Tellurium trace
less than 10 ppm and are used to quality control of Na131I solution using in medical
application.

I. Introduction
Na131I solution is prepared in the Center for Research and Raioisotope
Production by dry distillation method from irradiated Tellurium dioxide. This solution
can be contaminated Tellurium while international pharmacopeias only accepted
Tellurium content less than 10 ppm. For this reason, we have to study analytical
methods to control Tellurium content in final Na131I solution product using in medical
purposes produced at the Dalat Nuclear Research Institute by three methods that are spot
test, gamma spectrometric and spectrophotometeric methods.
II. The analysis methods
1. Determination of Tellurium in Na131I solution by spot test method
a. Preparation of reagents:
- Stannous chloride solution 5.0% (fresh preparation): Stannous chloride
dehydrate (SnCl2.2H2O) 0.25 g is dissolved in 0.25ml of concentrated hydrochloric acid,
heated to the clear solution and diluted to 5 ml with distilled water.
- Sodium hydroxide solution 25.0%: Sodium hydroxide 25 g is dissolved in
100 ml of distilled water.
- Standard Tellurium solution 10.0ppm: Stock solution of Tellurium 1,000 ppm
is prepared by dissolving 125.0862 mg of Tellurium dioxide in 2.7 ml of 25% sodium
hydroxide and to make the volume to 100 ml by distilled water. The stock solution is
diluted with distilled water to prepare the standard solution with concentration 10.0 ppm.
b. Chemical reaction:
SnCl2 + NaOH (c) = Na[Sn(OH)3] + 2NaCl
Na2TeO3 + 2Na[Sn(OH)3] + 3H2O = Te + 2Na2[Sn(OH)6]
c. The optimal conditions of determination of Tellurium content by spot test
method are investigated as below:
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VAEC-AR 06--33

Concentration of stannous chloride solution was 5.0%

Concentration of sodium hydroxide solution was 25.0%
Reaction time was 10 minutes.

d. Procedure:
- Place two drops (100 l ) of standard Tellurium solution, water (blank) and
sodium iodide (sample) solution into hole of spot plate.
- Add two drops (100 l ) of stannous chloride solution 5.0%, saturated sodium
carbonate and 25% sodium hydroxide respectively.
- Compare the black precipitation of Tellurium metal from the sample with
standard Tellurium and blank samples (Te4+ is reduced by Sn2+ to give the black
Tellurium metal). If there is preservative such as sodium thiosulfate (Na2S2O3) in the
sample solution, it will give the dark brown precipitation together with Tellurium metal.
2. Determination of Tellurium in Na131I solution by gamma- spectrometric
method
a. Preparation of reagents: CCl4 solvent (p.A); HNO3 (7N); KI 1mg/ml;
Standard Tellurium solution 10.0ppm.
Target preparation: Tellurium standard was prepared by taking 0.12508 g TeO2
(p.A) in quartz ampoule. The Tellurium standard and production target in reactor
irradiation container were irradiated on the reactor in the similar irradiation conditions
with Thermal neutron flux was 2.1013 n.cm-2.s-1, irradiation time was 108 h, cooling time
was 48 h and irradiation position: neutron trap. The ampoule containing Tellurium
standard was taken in a beaker containing 2ml NaOH 25%, followed by bidistiled water
to make the volume to 100 ml. Its stock standard solution Te 1mg/ml. The stock solution
is diluted with distilled water to prepare the standard solution with concentration 10.0
ppm.
Instrumentation: gamma-ray emitters were counted on a gamma-ray
spectrometer MANGMX-PTN INAA in conjunction with semiconductor detector
GMX-30190 (ORTEC). Measurement and spectrum were processed by Gamma Vision
32 (ORTEC) calibrated energy, efficacy and calculated by relative method.
b. Extraction of iodine with tetracarbonchloride:
Tetracarbonchloride is found to be useful extractant for iodine in nitric acid. The
formation of I2 is described as follows:
2NaI +

4HNO3

I2 + 2NO2 + 2NaNO3 + 2 H2O

Tetracarbonchloride used was analytical grade or chemically pure as

necessary. The initial Tellurium concentration in Na131I was too small in the aqueous
phase. The addition of KI carrier is necessary to avoid ultra-dilution phenomenon. We
have studied optimal conditions for the iodine extraction and extraction procedure such
as carrier content, acid concentration and effect of iodine concentration, reaction time
and number of extraction times. Our optimal extraction procedure was given as follows:
Two and half ml of bidistilled water and 100l of Na131I solution were
transferred into a separatory funnel of 60 ml volume. 100 l solution of KI 1mg/ml as
the carrier were added, 2ml of HNO3 7N were added, followed by drop by drop

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(300l) of concentrated nitric acid into the funnel. The mixture is mixed well until
formation of the color solution and standed for 2 minutes (I- is oxidized to give I2). Two
ml CCl4 added into mixture in funnel and mix well for 2 minutes (first extraction time).
I2 is a mostly extracted from an aqueous phase into the organic phase. The under
solution layer is the organic rose pink color phase containing 131I2. The organic phase
containing 131I2 is separated. Second and third times are carried out by addition of 2,0 ml
CCl4 into the extraction funnel (for second extraction time). The separation of organic
phase is repeated as before. Third extraction time (1,0 ml CCl4) has be done as before.
The upper aqueous phase is radioactive Tellurium solution. This solution is stored in
penicilline bottle 8ml for gamma spectrometric and spectrophotometeric measurements.
Extraction percentage is calculated as follows:

nn
1

E = 100 100. = 100.1

no
1 + D Vdm

V H 2O

with D
= 85
I (CCl )/I (H O)
2
4 2 2
c. Determination of Tellurium in Na131I solution by gamma-spectrometric
method:
Two and half ml of bidistilled water and 100l of Na131I solution were
transferred into a separatory funnel of 60 ml volume. 100 l solution of KI 1mg/ml as
the carrier were added, 2ml of HNO3 7N were added, followed by drop by drop
(300l) of concentrated nitric acid into the funnel. two ml CCl4 for first extraction
time. The addition of CCl4 is two ml for second extraction time and 1 ml CCl4 for third
time. A 8 ml aliquot of the organic phase was taken for counting. The solution of Na131I
produced at the Center for Research and Radioisotope Production was processed as
Tellurium standard sample.

Fig. 1. The standard gamma spectrum of Te 10g/ml

Fig. 2. The gamma spectrum of Te after extracted I-131

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Fig. 3. The gamma spectrum of I-131 solution

3. Determination of Tellurium in Na131I solution by spectrophotometeric

methods
a.Reagents:
Te4+ 10mg/ml and 1mg/ml; Na2WO40,5%, H2SO46N, Polyvinylalcohol (PVA)
2%, Nile blue 0,5%. Spectrophotometer UV-VIS.
b. Chemical reaction:
Na2TeO3 + 12Na2WO4 + 11H2SO4 = Na4[TeW12O40] + 11Na2SO4 + 11H2O
NatrioecacvonframoTellua
C2H5
4

C2H5

NH2

+ [TeW 1 2 O 4 0 ] -4

H+

N B 4 [TeW 1 2 O 4 0 ]

N ileB lue (N B + )

c. The optimal conditions of created Te4+ - Nile Blue complex are investigated as
below:
D

Pho ha p thu cu a ph c va thuo c th NB

0.16
0.14
0.12
0.1
0.08
0.06
0.04
0.02
0

0.15

Ph c

0.15

NB

0.1

0.1

0.05
0.05

VH2 SO4(ml)

10

12

450

500

550

600

650

700

t (phu t)

0
0

14

Fig. 4. Medium of create complex

236

400

nm
750

Fig. 5. The max bsorb of Te4+

complex and NB

The Annual Report for 2006, VAEC

30

60

90

120

150

180

210

240

Fig. 6. The durability of Te 4+

complex

VAEC-AR 06--33

D
0.2

0.25

Ca n d i va ca n tre n cu a vie c xa c nh Te 4+

ng chuan cua Te
0.2

0.2

0.15

0.05
0

0.05

CI-(mg)

0
0

0.2

0.4

0.6

0.8

1.2

1.4

Fig. 7. The impact of [ I-] on Te4+

complex

R 2 = 0.9993

0.1

0.1

0.05

y = 0.002x - 0.0081

0.15

0.15

0.1

20

40

60

80

100

120

140

20

40

60

80

CTe+4
100

C Te+4

160

Fig. 8. The limitation of Te 4+

concentration

Fig. 9. The curve of Te 4+

standard

The use of Te(IV) - tungstate-basic dyes - PVA systems for the determination of
Tellurium has not been investigated so far. Experimentally it was found that Tellurium
can react with tungstate and basic dye such as Nile blue (NB) to form ion-complexes,
which was stable in the presence of PVA. This color reaction has very high sensitivity,
stability and selectivity. This has been used for the determination of trace amounts of
Tellurium in solution of Na131I with satisfactory results. In this annual report we have
given the studied results and analytical procedure as follows:
Spectral characteristics: the absorption spectra of reagent blank against water
and ion-association complex of Te(IV) with tungstate in presence of PVA are recorded.
The absorption maximum of the ion-association complex is at 580 nm for NB, the the
absorption maximum of the reagent blank at 644 nm for NB .
Effect of acidity: our experiments show the dependence of the absorbance of the
ion-association complex on the solution acidity. The optimum acidity is 6N sulfuric acid
for NB.
Effect of reagent concentration: The optimum concentration of sodium tungstate
solution is 0.5%. The optimum concentration of the basic dye (NB) is 0.5%.
Effect of reaction time and stability of the absorbance: Te(IV) can react with
tungstate to form a complex in 10 min at room temperature. The ion-association
complex is formed in 2 min and stable at room temperature. The stability of the
absorbance is as follows: at least 240 minutes for the NB system.
Effect of iodine concentration: iodine concentration more than 0.8 mg/ml will
affect to the absorbance.
d. Determination of Tellurium in Na131I solution by spectrophotometeric method
In order to determine Te content in I-131 solution (because Te content in sample
is too low) we add a exact content Te into analysis sample. The determination of Te
can be done by the standard scheme with Te content 20-80g.
Blank sample: 2.0ml of bidistilled water into 25.00ml flasks
Standard sample: 50; 75; 100; 125; 150; 175; 200l of standard solution Te4+
10mg/ml into 7 flasks 25.00ml
Analytical sample: 100l I-131 solution and 100l
10mg/ml into 25.00ml flasks

Standard solution Te4+

Add into the above flask 2.0ml of sodium Tungstate 0.5%, 6 ml sulfuric acid 6
N, 1 ml PVA 2% and NB 0.5%, and followed by water to make to 25.00ml and mix well
for 10 minutes. Standard concentrations were added in flash. After shacking manually,
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the mixture was allowed to stand for 10 min at room temperature. The absorbances were
measured in 1 cm curvet at 580 nm against blank solution and a calibration curve was
prepared. Unknown test solutions were determined directly using the graph or excel
program in computer.
III. Table of analytical result
Tellurium content of solution of Na131I by three analytical methods
Sample code

Content of Te (ppm)
Spot Test

Spectrophotometeric
method

Gamma spectrometeric
method

200306

2-5

3,63 0,15

4,85 0,73

170406

2-5

4,43 0,06

4,76 0,66

150506

2-5

4,26 0,02

4.55 0,57

170706

2-5

3,35 0,08

5,20 0,88

140806

2-5

4,67 0,32

4.90 0,35

180906

2-5

3.14 0,04

3.24 0,45

I1140906 (Hungary)

2-5

4,44 0,18

161006

1-4

3,54 0,15

I5101006 (Hungary)

2-4

2,36 0,17

141106

2-5

2,71 0,29

I 5071106 (Hungary)

1-3

2,60 0,11

3.87 0,52
4.90 0,67

IV. Conclution
In order to control quality of Natriiodide (I-131) radiophamaceutical produced in
Dalat Nuclear Research Institute, We have been studied and established three analytical
processes for determining Tellurium content in Natriiodide solution.
Strengths and weaknesses on methods, we viewed that the Gamma spectrum has
high sensivity and exact but spend more time than other methods. So the gamma
spectrometric method use for periodic control three months per once. The Spot test
method is suitable than others in quality control of I-131 radiopharmaceutical in a
product batch. This method can determine Te content in sample 1ppm. The process
has introduced (entered) basis standard of laboratory and apply often at Center for
Research and Production of Radioisotopes. The specphotometeric method only uses for
reference.
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[3]. Ju.Lurie. Hand book of analytical Chemistry. Translated from the Russian by
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