Ecological aspects of 99Mo/99mTc production at an electron accelerator
The present report deals with experimental investigations into possible processes of accumulation of radioactive by-products (RBPs) during 99Mo/99mTc production at an electron linac. Foils from natural molybdenum (a target) and a number of typical target setup materials (Al, Ti, Cu, Ta, Ni and sta...
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nasplib_isofts_kiev_ua-123456789-790702025-02-09T18:14:10Z Ecological aspects of 99Mo/99mTc production at an electron accelerator Екологічні аспекти виробництва 99Мо/99mТс на прискорювачі електронів Экологические аспекты производства 99Мо/99mТс на ускорителе электронов Dikiy, N.P. Lyashko, Yu.V. Uvarov, V.L. Shlyakhov, I.N. Malets, Eu.B. Применение ускоренных пучков The present report deals with experimental investigations into possible processes of accumulation of radioactive by-products (RBPs) during 99Mo/99mTc production at an electron linac. Foils from natural molybdenum (a target) and a number of typical target setup materials (Al, Ti, Cu, Ta, Ni and stainless steel) were chosen as an object of investigations. The generation of radionuclides in the samples was performed in identical conditions under secondary radiation (bremsstrahlung + photoneutrons) of the linac LU-20 in a typical range of electron energies from 24 to 34 MeV. Викладені результати експериментального дослідження можливих процесів наробітку побічних радіонуклідов при виробництві 99Мо/99mТс на прискорювачі електронів. Як об'єкт дослідження відібрані фольги з природного молібдену (мішень) і набору характерних конструкційних матеріалів (Al, Ti, Cu, Ta, Ni, а також нержавіюча сталь). Генерація радіонуклідів у зразках виконувалося в ідентичних умовах у полі вторинного випромінювання (гальмівне+фотонейтрони) прискорювача ЛП-20 у характерному діапазоні значень енергії електронів 24...34 МеВ. Изложены результаты экспериментального исследования возможных процессов наработки побочных радионуклидов при производстве 99Мо/99mТс на ускорителе электронов. В качестве объекта исследования отобраны фольги из природного молибдена (мишень) и набора характерных конструкционных материалов (Al, Ti, Cu, Ta, Ni, а также нержавеющая сталь). Генерация радионуклидов в образцах производилась в идентичных условиях в поле вторичного излучения (тормозное+фотонейтроны) ускорителя ЛУ-20 в характерном диапазоне значений энергии электронов 24...34 МэВ. Робота виконана за підтримкою НТЦУ, контракт № 2185 2004 Article Ecological aspects of 99Mo/99mTc production at an electron accelerator / N.P. Dikiy, Yu.V. Lyashko, V.L. Uvarov, I.N. Shlyakhov, Eu.B. Malets // Вопросы атомной науки и техники. — 2004. — № 1. — С. 191-193. — Бібліогр.: 6 назв. — англ. 1562-6016 PACS: 06.60.Mr, 07.85.-m, 07.88+y, 81.30.Hd, 81.70.Jb https://nasplib.isofts.kiev.ua/handle/123456789/79070 en Вопросы атомной науки и техники application/pdf Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| institution |
Digital Library of Periodicals of National Academy of Sciences of Ukraine |
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DSpace DC |
| language |
English |
| topic |
Применение ускоренных пучков Применение ускоренных пучков |
| spellingShingle |
Применение ускоренных пучков Применение ускоренных пучков Dikiy, N.P. Lyashko, Yu.V. Uvarov, V.L. Shlyakhov, I.N. Malets, Eu.B. Ecological aspects of 99Mo/99mTc production at an electron accelerator Вопросы атомной науки и техники |
| description |
The present report deals with experimental investigations into possible processes of accumulation of radioactive
by-products (RBPs) during 99Mo/99mTc production at an electron linac. Foils from natural molybdenum (a target) and
a number of typical target setup materials (Al, Ti, Cu, Ta, Ni and stainless steel) were chosen as an object of investigations. The generation of radionuclides in the samples was performed in identical conditions under secondary radiation (bremsstrahlung + photoneutrons) of the linac LU-20 in a typical range of electron energies from 24 to
34 MeV. |
| format |
Article |
| author |
Dikiy, N.P. Lyashko, Yu.V. Uvarov, V.L. Shlyakhov, I.N. Malets, Eu.B. |
| author_facet |
Dikiy, N.P. Lyashko, Yu.V. Uvarov, V.L. Shlyakhov, I.N. Malets, Eu.B. |
| author_sort |
Dikiy, N.P. |
| title |
Ecological aspects of 99Mo/99mTc production at an electron accelerator |
| title_short |
Ecological aspects of 99Mo/99mTc production at an electron accelerator |
| title_full |
Ecological aspects of 99Mo/99mTc production at an electron accelerator |
| title_fullStr |
Ecological aspects of 99Mo/99mTc production at an electron accelerator |
| title_full_unstemmed |
Ecological aspects of 99Mo/99mTc production at an electron accelerator |
| title_sort |
ecological aspects of 99mo/99mtc production at an electron accelerator |
| publisher |
Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| publishDate |
2004 |
| topic_facet |
Применение ускоренных пучков |
| url |
https://nasplib.isofts.kiev.ua/handle/123456789/79070 |
| citation_txt |
Ecological aspects of 99Mo/99mTc production at an electron accelerator
/ N.P. Dikiy, Yu.V. Lyashko, V.L. Uvarov, I.N. Shlyakhov, Eu.B. Malets // Вопросы атомной науки и техники. — 2004. — № 1. — С. 191-193. — Бібліогр.: 6 назв. — англ. |
| series |
Вопросы атомной науки и техники |
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| fulltext |
ECOLOGICAL ASPECTS OF 99Mo/99mTc PRODUCTION
AT AN ELECTRON ACCELERATOR
N.P. Dikiy, Yu.V. Lyashko, V.L. Uvarov, I.N. Shlyakhov
National Science Center “Kharkov Institute of Physics and Technology”,
61108, Kharkov, Ukraine;
E-mail: uvarov@kipt.kharkov.ua;
Eu.B. Malets
Kharkov State Pedagogical University
The present report deals with experimental investigations into possible processes of accumulation of radioactive
by-products (RBPs) during 99Mo/99mTc production at an electron linac. Foils from natural molybdenum (a target) and
a number of typical target setup materials (Al, Ti, Cu, Ta, Ni and stainless steel) were chosen as an object of investi-
gations. The generation of radionuclides in the samples was performed in identical conditions under secondary radi-
ation (bremsstrahlung + photoneutrons) of the linac LU-20 in a typical range of electron energies from 24 to
34 MeV.
PACS: 06.60.Mr, 07.85.-m, 07.88+y, 81.30.Hd, 81.70.Jb
1. INTRODUCTION
In modern practice, more than 8500 medical institu-
tions throughout the world are exploiting up to 20 000
gamma-chambers for diagnostics of diseases by the
scintigraphy method. More than 70% of the procedures
are carried out with the use of 99mTc (daughter product
of the 99Mo isotope) as a radioactive tracer. The main
body of 99Mo (up to 200 000 Ci per year with a steady
tendency to increase) is produced in nuclear reactors
with the use of 235U fission reactions. In this case, only
6% of the reactions are accompanied by the production
of 99Mo. As a result, this method gives up to 50 Ci of ra-
dioactive waste (RAW) per 1 Ci of 99mTc, including
long-lived RBPs [2]. In view of the annual growth of
99Mo production and the absence of immediate prospect
of replacing 99mTc by another diagnostic radionuclide,
there arises the necessity of creating a new process of
99Mo/99mTc production with a less ecological load. This
technology based on the use of a high-current electron
accelerator has been developed (see ref. [3]) and is now
being promoted at KIPT.
2. SOURCES OF RBPs
By new technology, the converter, the target sub-
stance comprising 100Mo, and also the devices which ac-
commodate them serve as RBPs sources. The composi-
tion of RBPs and the rate of their generation are deter-
mined by the energy and value of the electron flow, by
the isotopic composition of the mentioned structures,
and also by their geometry with respect to the secondary
radiation field. In this case, only those active products
that are not retrapped into the production cycle can be
considered as RAW. These are the waste resulting from
the process of target treatment, 99mTc discharges (for the
most part, liquid), and also the spent constructives (sol-
id-state RAW).
The technology developed here provides for applica-
tion of different-type solid targets (metallic Mo or
MoO3 oxide) or liquid targets based on water solutions
of molybdenum acid salts, with molybdenum being of
both natural composition and enriched in the 100Mo iso-
tope. In view of relatively low total (up to 3 Ci) and spe-
cific (≤0.1 Ci/g) activities of the irradiated target, the
methyl ethyl ketone extraction of 99mTc (e.g., see refs.
[4,5]) has appeared the most acceptable method for ex-
traction of 99mTc. In the natural molybdenum case as a
target, the spent water phase (at the end of the week-
term technological cycle) is the main type of waste.
3. LIQUID TARGET
As it has become obvious from the studies, the liq-
uid target variant is most easily producible [6]. To in-
vestigate regularities in the liquid-phase generation of
99Mo and RBPs, a target device prototype was devel-
oped (Fig.1).
V2 V3 V4
e-
H2O
V1
γ
γ
γ
n
n
n
n
n
Mo
C
Fig. 1. Schematic of experiment to investigate the pro-
duction of 99Mo and RBPs in a liquid target
It includes a flowing water-cooled bremsstrahlung
converter C. Immediately behind the converter there is a
cylindrical vessel (V1), 80 mm in diameter and 40 mm
in height, which is axially symmetric to the electron
beam. Then sequentially follow a vessel, 32 mm in di-
ameter and 60 mm high (V2), and two vessels (V3 and
V4), 100 mm in height.
After irradiation of the target at given conditions, 1
to 2 ml samples of solution were taken from the vessels
and were directed for the analysis of induced activity by
means of the Ge(Li) detector. Tables 1 and 2 give the
results of the analysis of partial activity of targets based
on water solutions of Na2MoO4 salts (comprising
142 mg/ml of natural Mo) and K2MoO4 (208 mg/ml).
___________________________________________________________
PROBLEMS OF ATOMIC SIENCE AND TECHNOLOGY. 2004. № 1.
Series: Nuclear Physics Investigations (42), p.191-193. 191
4. SOLID TARGET AND CONSTRUCTIVES
To investigate the processes of RBPs generation in
structural materials of the target facility, samples of
most typical materials (Al, Ti, Cu, Ta, Ni, Mo and stain-
less steel) were chosen in the form of foils. The foils
were assembled as a sandwich and placed directly be-
hind the bremsstrahlung converter.
Table 1. Volumic activity (A) of isotopes in liquid target
vessels (Na2MoO4, 1 hour, 10 µA)
Е0,
MeV
№
v.
A, nCi/ml
90Mo 96Nb 99Mo 22Na 24Na
24
1 1.58 6.67 156.12 2.46 44.05
2 3.52 11.78 183.59 3.32 9.71
3 1.60 5.23 77.30 2.11 1.57
4 0.75 2.45 30.42 1.94 0.86
28
1 8.84 30.96 264.43 3.19 88.12
2 20.47 46.76 371.45 4.87 23.44
3 9.58 17.66 141.35 1.23 3.07
4 4.59 6.84 57.49 0.29 1.51
34
1 48.72 52.52 452.56 4.44 106.66
2 76.16 54.72 404.72 6.74 18.61
3 38.36 30.49 173.37 3.68 5.54
4 16.13 13.85 62.61 1.45 3.11
Table 2. Volumic activity of isotopes in target vessels
(K2MoO4)
E0,
MeV
№
v.
A, nCi/ml
90Mo 96Nb 99Mo
24
1 - 13,18 293,93
2 - 23,66 386,40
3 - 9,80 139,43
4 - 4,25 61,22
28
1 - 40,89 458,00
2 - 79,30 659,74
3 - 26,32 246,68
4 - 10,68 91,64
34
1 86,19 93,18 623,81
2 211,33 119,15 947,52
3 98,33 62,40 346,71
4 92,67 24,70 134,55
The accelerator LU-20 was operated in the mode of
direct (unscanned) beam, the parameters of which are
similar to the parameters described above. After irradia-
tion the foils were forwarded for the measurement of
their partial activity by means of the Ge(Li) spectrome-
ter. Table 3 lists the measured values of RBPs genera-
tion in the chosen set of structural materials and in natu-
ral Mo.
The columns of the table contain the following in-
formation: 1 - modes of target irradiation at accelerated
electron energies of 24 MeV (mode I), 28 MeV (mode
II) and 34 (mode III), the average accelerator current be-
ing 10 µA, 2 - basic reaction, 3 - half-life T1/2 of the ra-
dionuclide produced (days), 4 - specific partial activity
of radionuclide in the sample, 5 - iAmax is the estimated
maximum activity of the i- radionuclide in the techno-
logical cycle (300 µA, 24 hours), 6 - iAmax/ Mo-99Amax is
the ratio of iAmax to the maximum activity of generated
Mo-99.
The maximum activity of RBPs in the technological
cycle, iAmax, was estimated in the assumption that the
given material is concentrated in the infinite layer of
thickness (µρ)-1, where µ is the attenuation coefficient
of braking photons in the material, the photon energy
being in the region of photonuclear reaction, ρ is the
density of material.
For mode III (its conditions in the electron energy
are the closest to the ones realized in the technological
process), Table 4 gives both the calculated values of
RBPs activity accounted for by 5 Ci of the generated
99Mo immediately after completion of target irradiation,
and the data obtained from RBPs residual activity (total
Ai and gamma Ai
γ) at the end of the 5-day technological
cycle.
Table 3. Generation of basic radionuclides in structural
elements of the target facility
1 2 3 4(kBq
/g)
5(Ci) 6(Ci/
/Ci)
I
100Mo(γ,n)
→99Mo
2.75 54,4 3,24 1
48Ti(γ,p)
47Sc
3.35 19,5 1,27 0,39
58Ni(γ,n)57Ni
58Ni(γ,p)
→57Co
270.9 102,3 7,48 2,3
181Ta(n,γ)
→182Ta
115.0 0,260 0,00586 0,0018
65Cu(γ,n)
→64Cu
0.53 644 38,7 11,9
II
100Mo(γ,n)
→99Mo
2.75 80,8 4,53 1
48Ti(γ,p)
→47Sc
3.35 54,8 3,68 0,81
58Ni(γ,n)57Ni
58Ni(γ,p)
→57Co
270.9 204,7 14,5 3,28
181Ta(n,γ)
→182Ta
115.0 0,357 0,00838 0,00184
65Cu(γ,n)
→64Cu
0.53 1195 75,5 16,65
III
100Mo(γ,n)
→99Mo
2.75 103,0 5,87 1
48Ti(γ,p)
→47Sc
3.35 103,6 7,04 1,2
58Ni(γ,n)57Ni
58Ni(γ,p)
→57Co
270.9 298,3 21,4 3,65
181Ta(n,γ)
→182Ta
115.0 0,457 0,01089 0,00185
65Cu(γ,n)
→64Cu
0.53 1545 94,5 16,1
5. DISCUSSION
The analysis of the present data shows that the
equivalent dose rate (EDR) at the maximum of its distri-
bution on the surface of the samples under study is ap-
proximately proportional to the activity of radionuclides
produced in them as a result of irradiation, and increases
with electron energy in all cases. The data make it pos-
sible to make the proper choice for the target facility
components. The last ones should give the minimum
contribution to the total EDR of the radiated target setup
as compared with the radiation of the Mo target itself,
and also to produce mainly short-lived radionuclides.
The identical yield ratios of the 99Mo, 57Ni and 47Sc
isotopes in the samples from natural Mo, Ni and Ti for
different modes of irradiation have appeared the same as
in the stainless steel samples comprising similar ele-
ments. 57Ni is found to be the main source of induced
activity in stainless steel.
192
Table 4. Activity of basic RBPs in the technological cy-
cle
Iso-
top
Ai/5CiMo-99,
mCi
Аi after 5
days,mСi
Аγ
i after5
days,mСi
95mNb 2600 651 635
95Nb 3.1 26.9 26.9
88Zr 3.15 2.97 2.88
92mNb 8.0 4.9 4.9
96Nb 730 4.2 ∼4.2
91mNb 160 148 4.5
The data on the radionuclide yields in different ma-
terials (iAmax) at a target thickness equal to the mean
path of photons having the energy in the excitation re-
gion of the corresponding photonuclear reaction should
be considered as certain ultimate estimates. In particu-
lar, at a material thickness d << (µρ)-1 the produced ac-
tivity is Ai ~di⋅µ⋅ρ⋅ iAmax << iAmax. Besides, if the given
material is located in the target facility behind the Mo
target of thickness (µρ)-1, then the maximum yield of
side radionuclides is reduced by a factor of about e.
The measurement of surface activity distribution of
foils by the collimated radiometry method makes it pos-
sible to determine geometrical characteristics of the re-
gion of generation of different radionuclides and thus to
characterize the beam quality for the isotope production
process, and also to optimize the geometry and the ele-
mental composition of the target facility.
6. CONCLUSION
Methods have been developed and studies have been
made into the generation of radionuclides in targets and
structural materials at production of 99Mo/99mTc on the
electron accelerator. The photonuclear channel was the
main channel of radionuclide generation. The effect of
photoneutrons may manifest itself only in the reactions
98Mo(n,γ)99Mo, 92Mo(n,p)92mNb, 181Ta(n,γ)182Ta and
23Na(n,γ)24Na.
Among the structural elements under study, 54Mn
has the longest half-life (312.3 days). As regards the ac-
tivity produced, the use of such materials as Ni, Cu and
stainless steel is found to be the least desirable.
The data obtained on the yields of side radionuclides
with respect to the yield of 99Mo in the case of natural
Mo-based target are independent of the phase composi-
tion of the target (metal, solution or trioxide). These
data are required for the calculation of biological shield
of the “hot” chamber, which accommodates the extrac-
tion generator of 99mTc, and also, the vessel-collector for
liquid radioactive waste.
The results of determining the radionuclide compo-
sition of irradiated materials and their activity with due
regard for possible optimization of target facility materi-
als and geometry give evidence for considerable advan-
tages of the proposed technology of 99Mo/99mTc produc-
tion in relation to the ecology load.
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Atlanta, USA, Aug. 1994.
3. N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov. Funda-
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ЭКОЛОГИЧЕСКИЕ АСПЕКТЫ ПРОИЗВОДСТВА 99Мо/99mТс НА УСКОРИТЕЛЕ ЭЛЕКТРОНОВ
Н.П. Дикий, Ю.В. Ляшко, В.Л. Уваров, И.Н. Шляхов, Е.Б. Малец
Изложены результаты экспериментального исследования возможных процессов наработки побочных ра-
дионуклидов при производстве 99Мо/99mТс на ускорителе электронов. В качестве объекта исследования ото-
браны фольги из природного молибдена (мишень) и набора характерных конструкционных материалов (Al,
Ti, Cu, Ta, Ni, а также нержавеющая сталь). Генерация радионуклидов в образцах производилась в идентич-
ных условиях в поле вторичного излучения (тормозное+фотонейтроны) ускорителя ЛУ-20 в характерном
диапазоне значений энергии электронов 24...34 МэВ.
Работа выполнена при поддержке НТЦУ, контракт № 2185
ЕКОЛОГІЧНІ АСПЕКТИ ВИРОБНИЦТВА 99Мо/99mТс НА ПРИСКОРЮВАЧІ ЕЛЕКТРОНІВ
М.П. Дикий, Ю.В. Ляшко, В.Л. Уваров, І.М. Шляхов, Є.Б. Малец
Викладені результати експериментального дослідження можливих процесів наробітку побічних радіону-
клідов при виробництві 99Мо/99mТс на прискорювачі електронів. Як об'єкт дослідження відібрані фольги з
природного молібдену (мішень) і набору характерних конструкційних матеріалів (Al, Ti, Cu, Ta, Ni, а також
нержавіюча сталь). Генерація радіонуклідів у зразках виконувалося в ідентичних умовах у полі вторинного
випромінювання (гальмівне+фотонейтрони) прискорювача ЛП-20 у характерному діапазоні значень енергії
електронів 24...34 МеВ.
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PROBLEMS OF ATOMIC SIENCE AND TECHNOLOGY. 2004. № 1.
Series: Nuclear Physics Investigations (42), p.191-193. 193
Робота виконана за підтримкою НТЦУ, контракт № 2185
194
N.P. Dikiy, Yu.V. Lyashko, V.L. Uvarov, I.N. Shlyakhov
National Science Center “Kharkov Institute of Physics and Technology”,
61108, Kharkov, Ukraine;
E-mail: uvarov@kipt.kharkov.ua;
1. INTRODUCTION
3. LIQUID TARGET
4. SOLID TARGET AND CONSTRUCTIVES
A, nCi/ml
Isotop
REFERENCES
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