Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd
The results of experimental data analysis about the accumulation routes of the important medical isotope ¹⁰³Pd induced by charged particle beams (protons, deuterons, helium-3, helium-4) and neutral particles (gamma and neutrons) are presented. The main generalized data about the nuclear reaction cro...
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України
2023
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| Cite this: | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd / V.O. Hryhorenko // Problems of Atomic Science and Technology. — 2023. — № 3. — С. 66-71. — Бібліогр.: 24 назв. — англ. |
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| author | Hryhorenko, V.O. |
| author_facet | Hryhorenko, V.O. |
| citation_txt | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd / V.O. Hryhorenko // Problems of Atomic Science and Technology. — 2023. — № 3. — С. 66-71. — Бібліогр.: 24 назв. — англ. |
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| container_title | Problems of Atomic Science and Technology |
| description | The results of experimental data analysis about the accumulation routes of the important medical isotope ¹⁰³Pd induced by charged particle beams (protons, deuterons, helium-3, helium-4) and neutral particles (gamma and neutrons) are presented. The main generalized data about the nuclear reaction cross-section of ¹⁰³Pd production versus the irradiation techniques of natural and isotope-enriched targets and their content of unwanted accompanying radio nuclides were compared to theoretical predictions of too. The optimization procedure of the ¹⁰³Pd accumulation is discussed in order to develop more promising ones, taking into account the requirements for the production of medical radioisotopes.
Представлено результати аналізу експериментальних даних з накопичення важливого медичного ізотопу ¹⁰³Pd при використанні пучків заряджених частинок (протонів, дейтронів, гелію-3, гелію-4) та нейтральних частинок (гамма та нейтронів). Отримані узагальнені дані з активаційних виходів ¹⁰³Pd у залежності від методики опромінення натуральних та ізотопно-збагачених мішеней і вмісту в них небажаних супутніх радіонуклідів. Обговорюються шляхи оптимізації накопичення ¹⁰³Pd з метою пошуку більш перспективних з урахуванням вимог виробництва медичних радіоізотопів.
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| first_indexed | 2025-12-07T17:03:26Z |
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66 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145)
https://doi.org/10.46813/2023-145-066
CHARGED AND NEUTRAL PARTICLES BEAMS APPLICATION
FOR RESEARCH OF ACCUMULATION ROUTES OF THE MEDICAL
RADIOISOTOPE
103
Pd
V.O. Hryhorenko
Institute of High Energy Physics and Nuclear Physics
of the NSC “Kharkov Institute of Physics and Technology”, Kharkiv, Ukraine
E-mail: grigorenkovadim6@gmail.com
The results of experimental data analysis about the accumulation routes of the important medical isotope
103
Pd
induced by charged particle beams (protons, deuterons, helium-3, helium-4) and neutral particles (gamma and
neutrons) are presented. The main generalized data about the nuclear reaction cross-section of
103
Pd production
versus the irradiation techniques of natural and isotope-enriched targets and their content of unwanted
accompanying radio nuclides were compared to theoretical predictions of too. The optimization procedure of the
103
Pd accumulation is discussed in order to develop more promising ones, taking into account the requirements for
the production of medical radioisotopes.
PACS: 01.30.Rr; 29.85.Ca; 87.56.bg
INTRODUCTION
The medical isotope
103
Pd is widely used in the
treatment of oncological diseases, for example in
brachytherapy. The basis of which is the radiation
source placement directly in the affected tissue. Also,
the radioisotope
103
Pd is widely used for the treatment of
prostate cancer. Its application is more acceptable than
the isotope
125
I for this due to its emission properties:
T1/2=16.99 d, 186 Auger electrons, 95 conversion
electrons, about 80 X-rays per each 100 electron capture
decays, absence of high-energy -rays. Also,
103
Pd is
considered promising for Auger therapy. That’s why
new routes research of accumulating and optimizing
existing ones is an important and complex task.
The reaction cross section is important for
estimating the reaction yield [1]. In the case when the
research radioisotope is produced in various nuclear
reactions, including the daughter isotopes production by
decay, the cross sections of all production reactions can
be present like a sum (provided that T1/2 is significantly
less than that of the research isotope). In case of
reactions on different isotopes of the same target
chemical element, the cross sections can be added by
multiplying by the relative content of each isotope.
Thus, it is necessary to take into account the all cross-
sections of isotopes production from the decay chain of
the research isotope. Part of the left decay chain for
103
Pd [2] is shown in Fig. 1.
For medical application of
103
Pd, such main final
product requirements are presented [3]: the radionuclide
purity more than 99.95%, and the specific activity
≥50 Сi/g. In general, to increase the final nuclear
reaction yield, it is necessary either to increase the
charge particle beam current value, or to find another
nuclear reaction with a larger value of the production
cross-section. Accumulation of unwanted concomitant
isotopes usually also has to be considered. For example,
in our case
100
Pd (T1/2 = 3.63 days), which difficult to
separate from
103
Pd, which prevents its medical
application due to intense gamma radiation.
Fig. 1. Decay chain of
103
Pd radioisotope
Thus, the main requirements for optimizing the
accumulation routes of radioisotopes should be taken
into account:
• Selecting the isotopic composition of the target and
the type of incident particle to increase the nuclear
reaction yield;
• Approachability of incident particle beams
application, with relevant energy and beam currents
ranges for modern irradiation facilities;
• Inexpensive target material, simple chemical
treatment of the target after irradiation with minimal
losses;
• Reducing the nuclear reaction yields of unwanted
isotopes for accordance of specific activity and purity
requirements.
For the study of
103
Pd experimental yields from
different reactions, their cross section values
comparison is important and informative. Among the
experimental techniques of nuclear reaction yields
measurements depending the primary beam energy the
stack thin foil technique is highlighted. This approach
greatly simplifies the operational modes of charged
particle accelerators, but it is characterized by the
presence of primary beam losses during irradiation
process, as well as difficulties in measuring activity due
to X-ray self-absorption and the very weak intensity of
103
Pd X-rays. Therefore, it was previously decided to
ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145) 67
apply the TALYS [4] version 1.96 computer code
predictions to research for possible routes of
103
Pd
accumulation. In practice the theoretical predictions of
the dependence of the cross section (accumulation of the
studied isotope) depending the primary particle beam
energy for default mode, and compare it with available
experimental or another theoretical model predictions of
research nuclear reaction cross-section.
1. CHARGED PARTICLE BEAMS
APPLICATIONS
For medical isotope accumulation, cyclotron particle
accelerators are generally widely used, which are
usually optimized for this purpose and provided stability
and long-term operation during irradiation by requested
accelerated ion beam current and energy range.
Currently, the general route of accumulating [5]
103
Pd is the irradiation of a rhodium target by 18 MeV
proton beam of cyclotron irradiation facilities (in this
case maximum cross-section value is 600 mb). Such
facilities are widely used for the production of isotopes
for Positron Emission Tomography. The route
advantages are the high availability of such irradiation
devices in the world, high specific activity, and the
absence of unwanted radionuclide production.
Disadvantages include the presented not enough high
accelerated ion beam energy range which, accordingly,
does not allow increasing the activation yield (since the
thickness of the rhodium samples is ~0.05 cm as usual).
It should also be taken into account that rhodium is an
expensive target material.
An alternative route of
103
Pd accumulation is the
accelerated helium ion beam application with energies
up to 30 MeV [6]. A comparison of the experimental
cross sections [5–7] induced by protons and helium with
the theoretical prediction is presented in Fig. 2.
Fig. 2. Cumulative cross sections of
103
Pd and
100
Pd
production for nuclear reactions of protons and heliums
interactions with
103
Rh
It should be noted that there are a number of
discrepancies both between experimental data and
between experimental and calculated data. The
calculated activation yield for a thick
103
Rh target for
18 MeV proton beam energy is 8.02 MBq/(μA·h).
Instead, the experimental activation yield values are
10.24 MBq/(μA·h) measured by Hermanne et al. [5],
and Sudár et al. [7] – 8.1 MBq/(μA·h). There is also a
discrepancy between the experimental and calculated
activation yields for helium beam application. The
existing discrepancy requires a more detailed
experimental study of the accumulation of
103
Pd since
the most promising route is helium beam application
with an energy of up to 30 MeV.
Similar inconsistencies are also observed in the
analysis of experimental data for deuteron beam
application [8–10] and Rh target. The experimental data
do not have significant deviations, but have a large
discrepancy with the calculated data (Fig. 3). The
theoretical thick target activation yield for 40 MeV
incident deuteron beam energy equals
20.3 MBq/(μA·h), compared with 31.4 MBq/(μA·h)
measured by Hermanne et al. [8]. By the way, also
found differences between the results of calculated data
of Talys 1.2 and Talys 1.96 versions applications.
Fig. 3. Cumulative cross sections of
103
Pd and
100
Pd
production for the nuclear reactions of deuteron
interactions with
103
Rh
Another promising route of
103
Pd accumulation is
natural or enriched silver target application for high
energy proton beam interaction. The natural target is a
relatively cheap and consists only of two stable
isotopes:
107
Ag (51.8 %) and
109
Ag (48.2 %). The
corresponding dependencies of
103
Pd,
103
Ag and
100
Pd
production cross-sections [11–13] versus proton beam
energy are presented in Fig. 4.
Fig. 4. Cumulative cross sections of
103
Pd,
103
Ag and
100
Pd production for the nuclear reactions of proton
interactions with
nat
Ag target
68 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145)
The prediction of theoretical thick target activated
yield for protons with an energy of 78 MeV is equal to
37.26 MBq/(μA·h), but Uddin et al. [11] experimental
data for the same energy range is equal to
46.51 MBq/(μA·h).
Skakun and Qaim [14] measured and analyzed the
thick target activation yields of helions and α-particles
interactions with isotopically enriched Ru targets.
Experimental data of cross-sections of
103
Pd production
are shown in Fig. 5. The thick target activation yield is
equaled to 0.96 MBq/(μA·h) for the
100
Ru(α,n)
103
Pd
reaction at 25 MeV incident beam energy (theoretical
prediction value – 0.57 MBq/(μA·h)) and
1.05 MBq/(μA·h) for
101
Ru(a,2n)
103
Pd (0.76 MBq/μA·h)
at 23 MeV incident beam energy respectively.
Corresponding theoretical cross-section values are low
than experimental as usual. Proposed route applications
have strong limitations because the target material is
expensive.
Fig. 5. Cumulative cross sections of
103
Pd and
100
Pd
production for the nuclear reactions of helicon
and α-particles interactions with enriched Ru targets
Fig. 6. Cumulative cross sections of
103
Ag production
for the nuclear reactions of proton, helicon and α-
particles interactions with
nat
Pd target
Hermann et al. [8], Ditroi et al. [15], Ukon et
al. [16], and Aikawa et al. [17] studied nuclear reactions
induced by protons, deuterons, and α-particles with
nat
Pd
targets for
103
Ag production (T1/2=65.7 min). The main
idea is possibility to chemical extraction application of
103
Ag after accumulation process until it decays into
103
Pd. Corresponding cross-sections are presented in
Fig. 6 and Talys 1.96 prediction data for comparison
too.
In addition, TALYS 1.96 applying, the values of the
tritons interaction cross sections with natural silver and
rhodium targets (Fig. 7) for the accumulation of
103
Pd
were calculated. As results for 40 MeV tritons
103
Rh
thick target yield is 31 MBq/(μA·h). And triton energy
range to 25 MeV is more acceptable in comparison the
case
107
Ag application. There are no experimental data
about the discovered cross-section data. The main
problem is fast neutron yield increasing during long-
term experimental target irradiation for high-energy
tritium beam application.
Fig. 7. Cumulative cross sections of
103
Pd and
100
Pd
production for the nuclear reactions of tritons
interactions with
107
Ag and
103
Rh targets
2. NEUTRON ACTIVATION
For a long period, the leading position in the medical
isotopes production was occupied by nuclear
reactors [18]. Their application provide the
10
14
…10
15
n/(s·cm
2
) thermal neutron flux irradiation of
experimental samples with significant volumes.
Potentially, other sources can also be used for the
production of isotopes, for example [19] controlled by
ion accelerators with standard targets application of
light elements (such beryllium, lithium…). Nuclear
reactions (p,n), (d,n), (α,n) are usually used, but they
have a low efficiency (10
-2
n/particle [20]), respectively,
a relatively low neutron flux of 10
11
…10
12
n/s, which is
limited by accelerating ion current and difficulties with
target cooling.
The most compact neutron sources are also DT
generators, which are deuteron accelerators up to energy
~ 300 keV, and neutron energy ~ 14 MeV. Of cause,
they are not suitable for medical isotope production due
to the low neutron intensity ≥ 10
10
n/s for 4π
distributions. And also the strong limitation of their
operation (neutron production target lifetime) is present
too and close to several thousand hours depending on
the operation mode (direct, pulse…).
Intense electron accelerators of irradiation facilities
are also used as neutron sources, the bremsstrahlung
radiation of which is used to generate photoneutron
fluxes [21]. But it is well known that spallation sources
produce the highest neutron intensity among all types of
neutron generation facilities. For example, for SNS [22]
1 GeV accelerated proton beam with a current of
ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145) 69
1.5 mA interacts with a liquid mercury target. As a
result, the neutron production intensity is 10
17
n/s. Of
cause, high neutron production intensity is very
important for the medical isotope accumulation
technique providing. Production of high-energy neutron
flux by spallation source opens a new possibility for
medical isotope accumulation development.
For the accumulation of
103
Pd in the
102
Pd(n,γ)
103
Pd
reaction, the application of thermal neutrons was
considered as more effective. Natural palladium consists
of 6 isotopes:
102
Pd (1.02%),
104
Pd (11.14%),
105
Pd
(22.33%),
106
Pd (27.33%),
108
Pd (26.46%),
110
Pd
(11.72%). Provided the experimental target is enriched
with
102
Pd, a sufficient specific activity of 500 Ci/g [23]
produces during irradiation in the neutron reactor
irradiation facility with a relatively low content of
unwanted accompanying isotopes.
The average energy of fast neutrons in the reactor is
approximately 1…2 MeV. For the spallation neutron
source irradiation facility high energy (more than
45 MeV) neutron interactions with an enriched or
natural silver target could be discuss as a perspective
103
Pd accumulation route. Theoretical predictions of
according to the nuclear reaction cross-section are
presented in Fig. 8.
Fig. 8. Cumulative cross sections of
103
Pd production
for the nuclear reactions of high energy neutron
interactions with
107
Ag,
109
Ag and
nat
Ag targets
Fig. 9. Cumulative cross sections of
103
Pd production
for the nuclear reactions of fast neutron interactions
with stable palladium isotopes
For the case of
104
Pd enriched target application in
the
103
Pd accumulation route, it is sufficient to apply fast
neutrons with energy of up to 20 MeV. The calculated
cross-section data are presented in Fig. 9. The presented
data is characterized by the presence of a narrow
maximum, which requires the fulfillment of special
conditions during the irradiation and enrichment of
experimental palladium samples.
3. PHOTOACTIVATION
The generation of intense high-energy flux of γ-
quanta occurs due to the application of electron
accelerators, which, depending on the principle of their
formation, differ only in the spectral distribution of
energy (bremsstrahlung or Compton scattering).
For photoactivation technique as a route of
accumulating medical isotopes, there are certain
limitations associated with the mandatory isotopic
enrichment of the experimental target, the selection of
the optimal energy range of irradiation to ensure the
radioactive purity of the accumulated isotope, and the
influence of the background conditions associated with
the accompanying photoneutrons.
A detailed investigation of the
103
Pd accumulation
nuclear reactions in the interaction of γ-quanta with
stable isotopes of palladium has not yet been carried
out. Dikiy et al. [24] estimated the possibility of
103
Pd
accumulation. Natural targets were irradiated by fluxes
of bremsstrahlung and photoneutrons of 40 MeV
Electron Linac NSC KIPT. Integral an activation yield
of
103
Pd was experimentally determined. And it equals
to 4 μCi/(μA·h·g).
Taking into account Talys 1.96 predictions (Fig. 10)
of photonuclear reaction cross sections and
experimental data [24], it follows that optimization of
103
Pd accumulation in this case depends on gamma-
quanta energy range distributions, isotopic enrichment
of experimental targets and the neutron background
reduction during irradiation experiment. The application
of bremsstrahlung flux should not be considered
promising, but taking into account the regional features
of the placement of charged particle accelerators for the
development of medical isotopes, it is possible as an
additional one.
Рис. 10. The cross-section of
103
Pd production for the
nuclear reactions of gamma-quanta interactions with
natural isotopes of palladium
70 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145)
CONCLUSIONS
Preliminary data analysis on experimental and
theoretical values of nuclear reaction cross-sections is
presented. All of them applied or considered possible
for
103
Pd accumulation technology. The existing nuclear
data base of experimental cross-section requires deeper
analysis and comparison with theoretical predictions in
order to optimize computer codes, which will allow
more accurate prediction not only of nuclear reactions
of desired isotopes, but also of accompanying ones.
The main results of presented data about
103
Pd
accumulation routes are following that: isotopic
enrichment of any experimental samples for example
with
102
Pd (1.02% – natural distribution) or
104
Pd
(11.14%) makes any of the proposed routes of
accumulating
103
Pd more expensive.
It is an indisputable fact that, at present,
103
Rh
application as a target has advantages over all other
target materials. On the other hand, the accumulation of
the desired isotopes definitely depends on the
parameters of the beams and flux of primary particles,
namely their number in the required energy range.
The rapid development of accelerator facilities for
spallation neutron source provides to consider more
complex
103
Pd accumulation routes not only due to the
possibility of applying significant flux of fast neutrons.
In particular, it is necessary to carry out a more detailed
theoretical analysis taking into account fission reactions
as a promising accumulation of
103
Pd, for example,
nuclear reactions of
nat
Bi(n,f),
nat
Bi(γ,f) or
nat
Pb(n,f),
nat
Pb(γ,f). These elements are widely used in cooling
systems neutron production targets of many types of
spallation neutron sources.
ACKNOWLEDGEMENTS
The author would like to thank T.V. Malykhina as
the supervisor of my master's thesis, which was on a
similar topic, and S.H. Karpus for his consultation and
support during the work on this article.
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Article received 14.05.2023
ЗАСТОСУВАННЯ ПУЧКІВ ЗАРЯДЖЕНИХ ТА НЕЙТРАЛЬНИХ ЧАСТИНОК
ДЛЯ ДОСЛІДЖЕННЯ ШЛЯХІВ НАКОПИЧЕННЯ МЕДИЧНОГО РАДІОІЗОТОПУ
103
Pd
В.О. Григоренко
Представлено результати аналізу експериментальних даних з накопичення важливого медичного ізотопу
103
Pd при використанні пучків заряджених частинок (протонів, дейтронів, гелію-3, гелію-4) та нейтральних
частинок (гамма та нейтронів). Отримані узагальнені дані з активаційних виходів
103
Pd у залежності від
методики опромінення натуральних та ізотопно-збагачених мішеней і вмісту в них небажаних супутніх
радіонуклідів. Обговорюються шляхи оптимізації накопичення
103
Pd з метою пошуку більш перспективних з
урахуванням вимог виробництва медичних радіоізотопів.
https://doi.org/10.1016/j.apradiso.2007.11.013
https://doi.org/10.1016/j.apradiso.2017.07.049
https://doi.org/10.1016/j.nimb.2018.04.019
https://doi.org/10.1016/j.nimb.2019.04.066
https://doi.org/10.1016/j.physrep.2016.07.007
https://doi.org/10.1016/j.phpro.2014.11.024
https://doi.org/10.2172/1242669
|
| id | nasplib_isofts_kiev_ua-123456789-196142 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-07T17:03:26Z |
| publishDate | 2023 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Hryhorenko, V.O. 2023-12-10T16:53:52Z 2023-12-10T16:53:52Z 2023 Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd / V.O. Hryhorenko // Problems of Atomic Science and Technology. — 2023. — № 3. — С. 66-71. — Бібліогр.: 24 назв. — англ. 1562-6016 PACS: 01.30.Rr; 29.85.Ca; 87.56.bg DOI: https://doi.org/10.46813/2023-145-066 https://nasplib.isofts.kiev.ua/handle/123456789/196142 The results of experimental data analysis about the accumulation routes of the important medical isotope ¹⁰³Pd induced by charged particle beams (protons, deuterons, helium-3, helium-4) and neutral particles (gamma and neutrons) are presented. The main generalized data about the nuclear reaction cross-section of ¹⁰³Pd production versus the irradiation techniques of natural and isotope-enriched targets and their content of unwanted accompanying radio nuclides were compared to theoretical predictions of too. The optimization procedure of the ¹⁰³Pd accumulation is discussed in order to develop more promising ones, taking into account the requirements for the production of medical radioisotopes. Представлено результати аналізу експериментальних даних з накопичення важливого медичного ізотопу ¹⁰³Pd при використанні пучків заряджених частинок (протонів, дейтронів, гелію-3, гелію-4) та нейтральних частинок (гамма та нейтронів). Отримані узагальнені дані з активаційних виходів ¹⁰³Pd у залежності від методики опромінення натуральних та ізотопно-збагачених мішеней і вмісту в них небажаних супутніх радіонуклідів. Обговорюються шляхи оптимізації накопичення ¹⁰³Pd з метою пошуку більш перспективних з урахуванням вимог виробництва медичних радіоізотопів. The author would like to thank T.V. Malykhina as the supervisor of my master's thesis, which was on a similar topic, and S.H. Karpus for his consultation and support during the work on this article. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Problems of Atomic Science and Technology Application of nuclear methods Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd Застосування пучків заряджених та нейтральних частинок для дослідження шляхів накопичення медичного радіоізотопу ¹⁰³Pd Article published earlier |
| spellingShingle | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd Hryhorenko, V.O. Application of nuclear methods |
| title | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd |
| title_alt | Застосування пучків заряджених та нейтральних частинок для дослідження шляхів накопичення медичного радіоізотопу ¹⁰³Pd |
| title_full | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd |
| title_fullStr | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd |
| title_full_unstemmed | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd |
| title_short | Charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³Pd |
| title_sort | charged and neutral particles beams application for research of accumulation routes of the medical radioisotope ¹⁰³pd |
| topic | Application of nuclear methods |
| topic_facet | Application of nuclear methods |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/196142 |
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