J.RADIOANAL.NUCL.CHEM.

,LETTERS 127 /2/ 143-150 /19881

PRODUCTION OF IODINE-124 M

R.M. Lambrecht, M. Sajjad, M.A. Qureshi, S.J. Ai-Yanbawi

Radionuclide and Cyclotron Operation Department,

King Faisal Specialist Hospital and Research Centre,
P.O.Box 3354, Riyadh 11211, Kingdom of Saudi Arabia

Received 27 February 1988

Accepted 17 March 1988

Iodine-124 is produced in high yield by

the 124Te/d,2n/124I reaction and >99.5%
radionuclidic purity at 48 h post irradiation.
The production yield was 0.55+0.06 mCi/~Ah.
Radiochemical separation and ~argetry
methodology are described.

INTRODUCTION

Iodine-124 has appropriate physical characteristics

/T = 4.16d, B+ = 25%/ for its novel use in certain radio-
pharmaceuticals that can be utilized at low dose for PET
diagnostic evaluation of physiologic function, and at
high dose for radiotherapy I. Presently, 124I is only
mentioned as an unwanted impurity in the 123I products 2.
Iodine-124 can be produced by the 124Te/p,n/124I and
the 121Sb/~,n/124I reaction in very low yields 3'4. The
reported yields are 0.093 mCi/~Ah /Ref. 3/ and 1.05

XFor earlier papers in this s e r i e s see: R.M. Lambrecht

and M. Sajjad, Radiochimica Acta /in press/.

143 Elsevier Sequoia S. A., Lausanne

A kaddmiai Kiad6, Budapest
LAMBRECHT et al.: PRODUCTION OF IODINE-124

~Ci/~Ah /Ref. 4/, respectively. There is no reaction

reported in the literature by which 124I can be produced
in large quantities and high radionuclidic purity. Iodine-
124 can be produced in reasonable amount for labelling
purposes by the parameters for the production of radio-
pharmaceutical quality 124I.

EXPERIMENTAL

Irradiations

The features of the CS-30 cyclotron and its use at the

King Faisal Specialist Hospital and Research Centre have
5
been described elsewhere Iodine-124 is now routinely
produced using an internal target. The target is irradiat-
ed with a deuteron beam of 15 MeV energy. A specially de-
signed internal target assembly 6 for radionuclide produc-
tion accommodates a 124Te target for 124I production that
is stable for at least 6 h irradiations of 80-85 uA
/average/ beam currents. This permitted routine production
of ~250 mCi of 124I per run.

124Te targetry

The target consists typically of 130-160 mg of 95%

isotopically enriched 124Te that was electrodeposited on-
9
to a 16.15 cm- area of electroplated Ni on a Cu plate
/10.5 cm x 4.3 cm x 0.3 cm/. The Ni surface /%100 g.cm-2/
provided greatly increased adhesion for the electrode-
posited 124Te. Ni did not interfere in the radiochemical
separation.
7
The optimized technique for the preparation of tar-
gets for the 124Te/d,2n/124I reaction is comprised of
milling and lapping a Cu plate to uniform dimensional
specifications of the apparatus used to position the tar-
get matrix in hhe path of the accelerated deuterons. The

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 LAMBRECHT et al.: PRODUCTION OF IODINE-124

surface of the Cu plate is cleaned by sanding with 400

grade Carborundum, washed with distilled water, and
dried with an organic solvent. The Cu plate is placed in
a Ni plating solution prepared from nickel sulfate hexa-
hydrate /I.9M/. A platinum electrode was used as the anode
to electroplate on both sides of the Cu plate. The dry
weight of the Ni/Cu plate was determined after washing
the plate'with distilled water, organic solvent and dry-
ing at ii0 ~
The stock solution for electrodeposition of the iso-
topically enriched 124Te was typically prepared by con-
version of 2.5 g of 124Te to 124Te 0 2 in 35 ml of 8M HNO 3.
After evaporation to dryness, 124TEO2 was dissolved by
adding 2.8 g of KOH and 20 ml of water. The solution was
filtered to remove undissolved materials. The solution
was diluted to bring the KOH concentration to IM. It is
imperative that the 124Te plating solution be free of all
particulate matter prior to electrodeposition.

RADIOCHEMICAL PROCESSING

The method for the separation of iodide from telluri-

um was adapted from the reported methods 3'8'9 After ir-
radiation, the 124Te coating on the Cu/Ni target plate
was dissolved in a mixture of 1 ml 5M NaOH, 2 ml of 30%
H202 and deionized water as needed to cover 124Te depos-
it. After dissolution, the solution was transferred to
a flask containing 250 mg of aluminum powder. The target
plate and holder were rinsed three times with 5 ml of
water. Solution in the flask was heated gently until the
reaction was complete and all H202 was decomposed. Alu-
minum reduced Te/+IV/ to Te ~ Sometimes a dark violet
coloration was observed due to the formation of tellurides.

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LAMBRECHT et al.: PRODUCTION OF IODINE-124

Tellurides were o x i d i z e d to Te ~ b y streaming filtered

air. Filtered carbon dioxide gas was b u b b l e d through the
solution for 5 m i n A l u m i n u m was p r e c i p i t a t e d as the
hydroxide. The volume of the solution was reduced by
heating g e n t l y on a hot plate. After volume reduction,
CO 2 was b u b b l e d through the solution for a n o t h e r 5 min.
The solution was filtered through a glass frit into a
pre-weighed bottle. The gross weight of the stock
solution gave the total volu~e of the 124I solution.
The o v e r a l l radiochemical yield was t y p i c a l l y >90%
with a 1 h processing time. A fraction of the stock
solution was a s s a y e d on a Ge/Li/ detector calibrated
with a mixed primary standard o b t a i n e d from the U.S.
National B u r e a u of Standards.

The i s o t o p i c a l l y enriched 124Te M i x e d with a l u m i n u m

hydroxide was r e c o v e r e d from the glass frit and then
subsequently reused for the f a b r i c a t i o n of new targets.
I0 ii
The m e t h o d s of A c c e r b i et al. and Kondo et al. were
slightly modified. The p o w d e r was d i s s o l v e d in 7M HCI
containing 30% H202 /3:1 by volume/. The solution was
boiled to remove the excess of H202 and then c o n c e n t r a t -
ed HBr /5-10 ml/ was added. The solution was boiled to
reduce the volume. Deionized water was added to dilute
the solution by a factor of two. Hydrazine dihydro-
chloride was added until tellurium started to precipitate.
Finally, Na2SO 3 /5 g m / g m Te/ was added and the mixture
allowed to stand for 5 min, The solution was heated to
near boiling. The p r e c i p i t a t e was filtered through a
glass filter 0.45. The r e c o v e r e d 124Te was used to m a k e
n e w targets. The 124Te recovery was t y p i c a l l y %99.8%.

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 LAMBRECHT et al.: PRODUCTION OF IODINE-124

TABLE 1

Iodine-124 production yield data

Dose, Current, mCi/~Ah 124i,mC i 126i,mC i 124i, %

~Ah ~A (EOB) (EOB) (After 48 h)

iO0 25 0.56 57.0 0.5 99.1

200 25 0.60 i19.0 0.6 99.5
210 70 0.44 97.3 0.7 99.3
240 40 0.52 124.O 0.7 99.4
250 50 0.57 143.O 0.5 99.6"
300 60 0.59 150.O 0.6 99.6
325 65 0.62 201.O 1.3 99.3
500 75 0.48 260.0 1.2 99.5
500 80 0.54 269.7 1.8 99.3

RESULTS AND DISCUSSION

Table 1 summarizes the results for the production of

124I via 124Te/d,2n/124I reaction with 15 MeV deuterons
on 95% isotopically enriched 124Te. The source of 124Te
was Isotope Sales at Oak Ridge National Laboratory.
A series of targets were irradiated with 25 to 80 ~A
beam current. The production yield was proportional to
the dose. The plot /Fig. i/ of total yield vs. dose /~Ah/
gave a straight line of slope 0.55+--0.06 mCi]~Ah. The tar-
get integrity was maintained up to 6 h irradiation at
80 ~A with 15 MeV deuterons. The 124I production yiled
by the 124Te/d,2n/124I was found to be 0.55+0.06 mCi/~Ah.
This was much higher than 0.093 mCi/uAh obtained by the
124Te/p,n/1241 reaction iO . The 124Te /d,2n/ reaction is

also more convenient on the 15 MeV fixed energy CS-30

cyclotron, than use of the fixed energy 26 MeV proton

147
LAMBRECHTet al.: PRODUCTIONOF IODINE-124

y
260

240

'~,
~
200

160

120

80

40
-//
, I , I
0 200 400
Dose ,~Ah
Fig. i. Relationship of produced 124I and the dose on
target with 2 ~ - ~ . ~ A beam of 15 MeV deuterons
on 13+1 mg cm ~ ~=~Te

beam. The proton beam would have to be extracted and

degraded to about 13.5 MeV /Ref. 3/ in order to optimize
124
the yield and purity of I produced via the /p,n/ re-
action. The radionuclidic purity of 124I produced with
15 MeV deuterons on thin internal target was found to
be greater than 99.5% /see Table i/ provided the sample
was allowed to cool 48 h. The radionuclidic impurity
was 126I /T = 13.1 d/ after the coproduced 123I /T =
13.1 h/ and 1301 /T = 12.36 h/ had decayed. The 126I
may have been produced by the 0.93% 125Te isotopic im-
purity in the enriched 124Te target.
The radiochemical method was used for preparing 124~
labelled meta-iodobenzylguanidine 12 and is of interest
as a label for monoclonal antibodies 13 appropriate for
radioimmunotherapeutic agents 14. The quality control of
124I iodide solutions will be reported separately 15

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 LAMBRECHT et al.: PRODUCTION OF IODINE-124

This research was supported in part by a private grant

/RAC Project No. 85-0027/ from Sheik Abdulrahman All AI-
Jeraisy.

REFERENCES

i. R.M. Lambrecht, N. Woodhouse et al., Investigational

Study of Iodine-124 with a Positron Camera, Amer. J.
Physiol. Imaging /submitted/.

2. M. Berman, L.E. Braverman, J. Burke, L. De Groot,

K.R. McGornack, T.H. Oddie, R.H. Rohrer, N.H. Well-
man, E.M. Smith, J. Nucl. Med., 16 /1975/ 857.

3. K. Kondo, R.M. Lambrecht, A.P. Wolf, Intern. J. Appl.

Radiat. Isotopes, 28 /1977/ 395.

4. D.J. Silvester, J. Sugden, I.H. Watson, Radiochem.

Radioanal. Lett., 2 /1969/ 17.

5. J.W. Stetson, R.M. Lambrecht, M. Sajjad, F.W. Zielins-

ki, Proc. llth Int. Conf. on Cyclotron and Their
Applications, Ionics, Tokyo, 1986, pp. 678-681.

6. R.H. Syed, W. Meyers, M. Sajjad, R.M. Lambrecht, Nucl.

Instrum. and Methods /submitted/.

7. Standard Operating Procedures of the Rad• and

Cyclotron Operations Department, King Faisal Specialist
Hospital and Research Centre /unpublished/.

8. M.A. Qureshi, L. McIsaac, D. Schlyer, H.B. Hupf, F.A.H.

Ai-Watban, D. Lewall, Int. J. Nuc !. Med. Biol., 12
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9. H.B. Hupf, S.D. Tischer, F.A.H. Ai-Watban, Nucl. Instrum.

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iO. E. Acerbi, C. Birattari, M. Castiglioni, F. Resmini,

M. Villa, Intern. J. Appl. Radiat. Isotopes, 26
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ii. K. Kondo, R.M. Lambrecht, E.F. Norton, A.P. Wolf.

Intern. J. Appl. Radiat. Isotopes, 28 /1977/ 765.

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12. M.A. Qureshi, M, Sajjad, M.M. Vora, S.A. Bakr, R.M.

Lambrecht, H.Y, Aboul-Enein, D.F. Wolczak, Proc.
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Chemistry, Sydney, Vol. 2, 1987, pp. 223-227.

13. T. McGarry, R.M. Lambrecht, M. Ai-Ahdal, 2nd Int.

Conf. on Monoclonal Antibody Immunoconjugates for
Cancer, San Diego, CA, March 12-14, 1987.

14. R.M. Lambrecht, M. Sajjad, S.A. Bakr, 35th Annual

Meeting of the Society of Nuclear Medicine, June
14-17, 1988 /submitted/.

15. M. Sajjad, R.M. Lambrecht, S.A. Bakr, Int. J. Radiat..

Appl. Instrum. Part B. Nucl. Med. /submitted/.

150