On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin
The experiment-calculated method for separation of total α-activities of plutonium isotopes A(²³⁹Pu+²⁴⁰Pu) on partial activities A(²³⁹Pu) and A(²⁴⁰Pu) in emergency fallout of Chernobyl accident origin is developed. Розроблено розрахунково-експериментальний метод роздiлення сумарних α-активностей iзо...
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| Опубліковано в: : | Вопросы атомной науки и техники |
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| Дата: | 2009 |
| Автори: | , , , , |
| Формат: | Стаття |
| Мова: | Англійська |
| Опубліковано: |
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
2009
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| Назва журналу: | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| Цитувати: | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin / A.N. Vodin, S.N. Olejnik, E.A. Rudak, I.V. Ushakov, O.I. Yachnik // Вопросы атомной науки и техники. — 2009. — № 5. — С. 90-94. — Бібліогр.: 14 назв. — англ. |
Репозитарії
Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1859668462184431616 |
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| author | Vodin, A.N. Olejnik, S.N. Rudak, E.A. Ushakov, I.V. Yachnik, O.I. |
| author_facet | Vodin, A.N. Olejnik, S.N. Rudak, E.A. Ushakov, I.V. Yachnik, O.I. |
| citation_txt | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin / A.N. Vodin, S.N. Olejnik, E.A. Rudak, I.V. Ushakov, O.I. Yachnik // Вопросы атомной науки и техники. — 2009. — № 5. — С. 90-94. — Бібліогр.: 14 назв. — англ. |
| collection | DSpace DC |
| container_title | Вопросы атомной науки и техники |
| description | The experiment-calculated method for separation of total α-activities of plutonium isotopes A(²³⁹Pu+²⁴⁰Pu) on partial activities A(²³⁹Pu) and A(²⁴⁰Pu) in emergency fallout of Chernobyl accident origin is developed.
Розроблено розрахунково-експериментальний метод роздiлення сумарних α-активностей iзотопiв
плутонiю A(²³⁹Pu+²⁴⁰Pu) на парцiальнi α-активностi A(²³⁹Pu) та А(²⁴⁰Pu) в аварiйних випаданнях Чорнобильського походження.
Разработан расчетно-экспериментальный метод разделения суммарных α-активностей изотопов
плутония A(²³⁹Pu+²⁴⁰Pu) на парциальные α-активности A(²³⁹Pu) и А(²⁴⁰Pu) в аварийных выпадениях Чернобыльского происхождения.
|
| first_indexed | 2025-11-30T12:40:46Z |
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| fulltext |
ON POSSIBILITY OF SEPARATION OF 239Pu AND 240Pu
CONTRIBUTIONS IN EMERGENCY PLUTONIUM FALLOUT
OF CHERNOBYL ACCIDENT ORIGIN
A.N. Vodin1∗, S.N. Olejnik1, E.A. Rudak2, I.V. Ushakov1, O.I. Yachnik2
1National Science Center “Kharkov Institute of Physics and Technology”, 61108, Kharkov, Ukraine
2Institute of Physics, National Academy of Sciences of Belarus, Minsk, Belarus
(Received July 15, 2009)
The experiment-calculated method for separation of total α-activities of plutonium isotopes A(239Pu+240Pu) on
partial activities A(239Pu) and A(240Pu) in emergency fallout of Chernobyl accident origin is developed.
PACS: 28.41.Kw, 28.60.+s, 28.90.+i, 29.85.Fj
1. INTRODUCTION
It is known that 238Pu, 239Pu and 240Pu give the
main contribution to the total α-activity of pluto-
nium isotopes in emergency fallout of Chernobyl ac-
cident origin. Thus, for technical reasons, only the
total α-activity of 239Pu and 240Pu isotopes
A(239,240Pu) = A(239Pu) + A(240Pu)
is usually measured, and that reduces the useful-
ness of laborious and costly α-spectrometric measure-
ments.
It was previously shown [1], [2], that fission frag-
ments 103Ru and 106Ru can be used for indirect def-
inition of A(239,240Pu) and the activity ratio
ρ(Ru) = A(106Ru)/A(103Ru)
can have independent value for the estimation of fuel
burnout W . According to theoretical calculations [3],
[4], the relevant activity ratio is characterized by a
linear dependence on W :
ρ(Ru, W ) ≈ W/49.5.
And since the burnout W comply with the Poisson
distribution
PW = (< W >)W · e−<W>
W !
or the related Gaussian distribution
P (W )dW =
√
2π < W > · e−(W−<W >)2
2<W > dW,
the experimental yields of the activity ratio
ρ(Ru)exp = A(106Ru)/A(103Ru)
must also comply with the Poisson or Gaussian dis-
tribution.
In [3] by using the experimental data on soil
contamination of Mogilev region (the distance from
Chernobyl nuclear power plant (ChNPP) is about
200 km) and Bragin region (the distance from
ChNPP is about 50 km) it was shown that this is
really true. Since the ruthenium fell out mostly in
aerosol form in Mogilev region, and both in fuel and
aerosol form in Bragin region, it is clear that the ac-
tivity ratio of 103Ru and 106Ru does not depend on
the form of ruthenium fallout.
According to [1], [2], a similar situation should
occur for 239Pu and 240Pu since the activity ratio of
these isotopes is also characterized by a linear depen-
dence on W :
ρ(Pu,W ) = A(240Pu,W )/A(239Pu,W ) ≈ W/8.
This fact can be used to separate the contributions
of 239Pu and 240Pu isotopes in the total α-activity
A(239,240Pu). And that is the main purpose of this
work.
2. ANALYSIS OF EXPERIMENTAL DATA
ON SOIL CONTAMINATION SOUTH OF
GOMEL REGION
Since the activity ratios
ρ(Ru,W ) = A(106Ru,W )/A(103Ru,W )
and
ρ(Pu, W ) = A(240Pu,W )/A(239Pu,W )
similarly depend on W it is possible to eliminate an
explicit dependence of W and obtain the activity ra-
tio:
A(240Pu)/A(239Pu) = 6.2 · ρ(Ru), (1)
where ρ(Ru)=A(106Ru)/A(103Ru).
∗Corresponding author. E-mail address: vodin@kipt.kharkov.ua
90 PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY, 2009, N5.
Series: Nuclear Physics Investigations (52), p.90-94.
The ratio (1) should also be confirmed by exper-
imental data. Withal the right side of this ratio can
be reliably measured. Therefore the activity ratio of
A(240Pu) and A(239Pu)
A(240Pu) = 6.2 · ρ(Ru)exp ·A(239Pu) (2)
can be experimentally established. Based on (1) and
(2) the expressions for the partial activities A(239Pu)
and A(240Pu) can be obtained through the total ac-
tivity A(239,240Pu):
A(239Pu) = A(239,240Pu)
1
[1 + 6.2 · ρ(Ru)exp]
, (3)
A(240Pu) = A(239,240Pu)
6.2 · ρ(Ru)exp
[1 + 6.2 · ρ(Ru)exp]
. (4)
By using (3) and (4) the division of experimen-
tal data on plutonium 239Pu+240Pu contamination
of soil south of Gomel region can be performed.
The main experimental data on density of soil
contamination in Belarus by γ-emitting fission frag-
ments were obtained in [5]-[7]. Later they were sys-
tematized and formed the basis of the national data-
base.
The most complete experimental data on plu-
tonium 239Pu+240Pu contamination levels are con-
tained in [8], [9]. For the analysis 168 populated areas
were selected for which the data both for plutonium
and fission fragments were available.
As a result the experimental activity ratios
A(240Pu)/A(239Pu) were received. The diagram of
experimental yields of A(240Pu)/A(239Pu) is shown
in Fig.1.
Fig.1. Yields n(ρ)of experimental ratios
A(240Pu)/A(239Pu)
Qualitatively this diagram is well con-
formed to theoretical predictions for the ratio
A(240Pu)/A(239Pu). The average experimental value
is equal to < ρexp >≈ 1.37. Theoretical ratios are
well described by a function:
ρtheor = 0.122 + 23.7 · (e0.00483W − 1).
The average theoretical value at < W >= 11 is equal
to < ρtheor >≈ 1.4, i.e. practically coincides with the
experimental one.
It is obvious that the division of experimental val-
ues of α-activities A(239,240Pu) with help of the ratio
ρexp = A(106Ru)/A(103Ru) leads to reasonable re-
sults.
The partial experimental α-activities A(239Pu)
and A(240Pu) received can be used to analyze the
ratios like
ρ = A(239Pu)/A(X )
and
ρ = A(240Pu)/A(X ),
where X - fission fragments associated with the fuel
matrix (e.g., 95Zr, 141Ce, 144Ce) or fission fragments
with variable volatility (e.g., 103Ru, 106Ru).
3. EXPERIMENTAL ACTIVITY RATIOS
ρ = A1/A2
In relation to dependence of isotope production on
fuel burnout W the activities A(103Ru) and A(106Ru)
are analogues of A(239Pu) and A(240Pu), respectively.
According to theoretical calculations [3], [4], [10]:
A(239Pu) ≈ 2 · 10−4 ·A(103Ru)
and
A(240Pu) ≈ 1.36 · 10−3 ·A(106Ru).
Therefore, this fact can be used to establish the na-
ture of plutonium isotopes in Chernobyl fallout.
First let us consider the behavior of ruthenium
isotopes A(103Ru) and A(106Ru). It is known that
they are fission fragments with variable ¿volatileÀ (in
the terminology of [11]), i.e. they can fall out as nu-
clides associated with the fuel matrix (at relatively
small distances from ChNPP), and as aerosol com-
pounds (at large distances from ChNPP) (e.g., see
[11] and references therein). This fact should affect
the spectrum of experimental ratio yields, e.g.
ρ(103Ru,95 Zr) = A(103Ru)/A(95Zr)
and
ρ(106Ru,95 Zr) = A(106Ru)/A(95Zr).
Diagrams of experimental yields of ρ(103Ru,95Zr) and
ρ(106Ru, 95Zr) are shown in Fig.2 and Fig.3.
According to theoretical calculations, the average
values of the ratios at < W >= 11 are equal to
< ρ(103Ru,95 Zr)theor >≈ 0.75
and
< ρ(106Ru,95 Zr)theor >≈ 0.16.
That is 1.6 and 1.7 times less than the experimental
values
< ρ(103Ru,95 Zr)exp >≈ 1.2
and
< ρ(106Ru,95 Zr)exp >≈ 0.27,
respectively. While the peaks in distributions are
approximately located at the points where the the-
ory predicts. The average values of ratios increase
because of the ¿trailÀ smoothly decreasing towards
the large values.
91
Fig.2. Yields of the ratio ρ(103Ru,95Zr)
Fig.3. Yields of the ratio ρ(106Ru,95Zr)
Fig.4. Yields of the ratio ρ(239Pu,95Zr)
Fig.5. Yields of the ratio ρ(240Pu,95Zr)
Ruthenium isotopes 103Ru and 106Ru are nuclides
with variable ¿volatilityÀ, and 95Zr is associated
with the fuel matrix. Therefore, the increase in ra-
tios < ρ(103Ru,95Zr)exp > and < ρ(106Ru,95Zr)exp >
compared with the theoretical estimation can be ex-
plained only by ¿volatileÀ of the ruthenium.
It is obvious that if the ruthenium in the form of
aerosols and other species not associated with the fuel
matrix can be added to the fuel ruthenium, the ra-
tios < ρ(103Ru,95Zr)exp > and < ρ(106Ru,95Zr)exp >
only increase as compared to < ρ(103Ru,95Zr)theor >
and < ρ(106Ru,95Zr)theor >.
By analogy we can consider the experimental ra-
tios
ρ(239Pu,95 Zr) = A(239Pu)/A(95Zr)
and
ρ(240Pu,95 Zr) = A(240Pu)/A(95Zr).
Diagrams of experimental yields of ρ(239Pu,95Zr) and
ρ(240Pu,95Zr) are shown in Fig.4 and Fig.5.
According to theoretical calculations, the average
values of these ratios at < W >= 11 are equal to
< ρ(239Pu,95 Zr)theor >≈ 1.5 · 10−4
and
< ρ(240Pu,95 Zr)theor >≈ 2.1 · 10−4.
That is 2 times less than the corresponding experi-
mental values
< ρ(239Pu,95 Zr)exp >≈ 3 · 10−4
and
< ρ(240Pu,95 Zr)exp >≈ 4.1 · 10−4.
The situation is the same as in the case of ratios
< ρ(103Ru,95Zr)exp > and < ρ(106Ru,95Zr)exp > dis-
cussed earlier. The peaks in distributions are approx-
imately located at the points where the theory pre-
dicts. The average values of ratios increase because
of the ¿trailÀ smoothly decreasing towards the large
values too.
Therefore, we can assume that the ruthenium and
plutonium isotopes in Chernobyl fallout in the south
of Gomel region behave similarly. Thus, for the con-
sideration set of experimental data this confirms a
similar conclusion of [12],[13].
It is interesting to consider the ratios
ρ(239Pu,103Ru) and ρ(240Pu,106Ru) under the as-
sumption that the ruthenium and plutonium iso-
topes could fall out both as fuel and not associated
with the fuel forms. Diagrams of experimental yields
of ρ(239Pu,103Ru) and ρ(240Pu,106Ru) are shown in
Fig.6 and Fig.7.
As noted above, according to theoretical calcula-
tions
A(239Pu) ≈ 2 · 10−4 ·A(103Ru)
and
A(240Pu) ≈ 1.36 · 10−3 ·A(106Ru).
Therefore the average experimental values
< ρ(239Pu,103 Ru)exp >≈ 2.2 · 10−4
and
< ρ(240Pu,106 Ru)exp >≈ 1.4 · 10−3
92
practically coincide with theoretical estimates. Natu-
rally, this can only be if the ruthenium and plutonium
isotopes in Chernobyl fallout behave similarly.
Fig.6. Yields of the ratio ρ(239Pu,103Ru)
Fig.7. Yields of the ratio ρ(240Pu,106Ru)
However, the experimental values of
ρ(239Pu,103Ru) and ρ(240Pu,106Ru) are both left and
right of the average theoretical values
< ρ(239Pu,103 Ru)theor >≈ 2 · 10−4
and
< ρ(240Pu,106 Ru)theor >≈ 1.4 · 10−3.
It is easy to explain with the sorption of ruthe-
nium or plutonium isotopes in aerosol form by the
fuel particles with the ¿normalÀ average activity ra-
tios A(239Pu)/A(103Ru) and A(240Pu)/A(106Ru).
4. CONCLUSIONS
The main purpose of this work is the develop-
ment of the experiment-calculated method for sep-
aration of total α-activities of plutonium isotopes
A(239Pu+240Pu) on partial activities A(239Pu) and
A(240Pu) in emergency fallout of Chernobyl accident
origin. The method is based on the fact that radionu-
clide activities A(106Ru), A(239Pu) and A(240Pu) in
the active zone of the thermal reactor are closely as-
sociated with each other.
The 106Ru nuclide is generated mainly in the re-
action of fission of 239Pu by thermal neutrons. Its
production is approximately linear on the burnout
W and that is confirmed experimentally [14].
The 240Pu nuclide is also generated primarily on
239Pu but in the reaction of radioactive neutron cap-
ture. Its production is also proportional to W . Con-
sequently, the activity ratio A(240Pu)/A(106Ru) prac-
tically does not depend on W .
The productions of 239Pu and 103Ru in thermal
reactors do not have a direct genetic association.
However, the dependence of its activities on W in
the thermal reactor is similar.
The activity ratio A(239Pu)/A(103Ru), as in the
case of A(240Pu)/A(106Ru), practically does not de-
pend on W . In other words, a combination of activi-
ties
ρ(Ru,Pu) =
A(240Pu,W ) ·A(103Ru,W )
A(239Pu,W ) ·A(106Ru,W )
both in the active zone of a thermal reactor, and in
the emergency fallout does not depend on W , in par-
ticular, for the emergency high power channel reactor
HPChR-1000 ρ(Ru,Pu)≈0,16. This ratio was used to
analyze the experimental data on soil contamination
south of Gomel region by 239Pu+240Pu isotopes and
95Zr, 103Ru, 106Ru, 137Cs, 141Ce and 144Ce fission
fragments.
At the same time the data both on the local
burnout W values and on the partial α-activities
A(239Pu) and A(240Pu), which are more informa-
tive than the initial total α-activity A(239,240Pu),
were received. As a result, this allowed to ana-
lyze the experimental data on pairs of activity ra-
tios like A(239Pu)/A(XX) and A(240Pu)/A(XX),
A(103Ru)/A(XX) and A(106Ru)/A(XX).
The main conclusions are:
• Spectra of the experimental outputs of
A(239Pu)/A(XX) and A(103Ru)/A(XX),
A(240Pu)/A(XX) and A(106Ru)/A(XX) have
the same structure, where X - fission fragments
associated the fuel matrix 95Zr, 141Ce, 144Ce.
• The average experimental values of this ratios is
about 1.5 times more than the theoretical ones
for the fuel at the average value < W >= 11.
It should be noted that besides the ratios
ρ(Ru,Pu) =
A(240Pu,W ) ·A(103Ru,W )
A(239Pu,W ) ·A(106Ru,W )
,
there are other four activities with similar structure,
which can be useful in the analysis of soil contamina-
tion with plutonium isotopes. In particular,
A(239Pu, W ) ·A(240Pu,W )
A(103Ru, W ) ·A(106Ru, W )
≈ 2.6 · 10−7
also does not depend on the fuel burnout.
ACKNOWLEDGMENTS
This work was supported by the Ministry of Educa-
tion and Sciences of Ukraine (grant No. M/68-2008)
and the Byelorussian republican fund for fundamen-
tal researches (grant No. Φ09ΓKHT-003).
93
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О ВОЗМОЖНОСТИ РАЗДЕЛЕНИЯ ВКЛАДОВ 239Pu И 240Pu
В АВАРИЙНЫХ ВЫПАДЕНИЯХ ПЛУТОНИЯ ЧЕРНОБЫЛЬСКОГО
ПРОИСХОЖДЕНИЯ
А.Н. Водин, С.Н. Олейник, Э.А. Рудак, И.В. Ушаков, O.И. Ячник
Разработан расчетно-экспериментальный метод разделения суммарных α-активностей изотопов
плутония A(239Pu+240Pu) на парциальные α-активности A(239Pu) и А(240Pu) в аварийных выпаде-
ниях Чернобыльского происхождения.
ПРО МОЖЛИВIСТЬ РОЗДIЛЕННЯ ВНЕСКIВ 239Pu ТА 240Pu
В АВАРIЙНИХ ВИПАДАННЯХ ПЛУТОНIЮ ЧОРНОБИЛЬСЬКОГО
ПОХОДЖЕННЯ
О.М. Водiн, С.М Олiйник, Е.А. Рудак, I.В. Ушаков, O.I. Ячник
Розроблено розрахунково-експериментальний метод роздiлення сумарних α-активностей iзотопiв
плутонiю A(239Pu+240Pu) на парцiальнi α-активностi A(239Pu) та А(240Pu) в аварiйних випаданнях
Чорнобильського походження.
94
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| id | nasplib_isofts_kiev_ua-123456789-96513 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-11-30T12:40:46Z |
| publishDate | 2009 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Vodin, A.N. Olejnik, S.N. Rudak, E.A. Ushakov, I.V. Yachnik, O.I. 2016-03-17T20:47:12Z 2016-03-17T20:47:12Z 2009 On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin / A.N. Vodin, S.N. Olejnik, E.A. Rudak, I.V. Ushakov, O.I. Yachnik // Вопросы атомной науки и техники. — 2009. — № 5. — С. 90-94. — Бібліогр.: 14 назв. — англ. 1562-6016 PACS: 28.41.Kw, 28.60.+s, 28.90.+i, 29.85.Fj https://nasplib.isofts.kiev.ua/handle/123456789/96513 The experiment-calculated method for separation of total α-activities of plutonium isotopes A(²³⁹Pu+²⁴⁰Pu) on partial activities A(²³⁹Pu) and A(²⁴⁰Pu) in emergency fallout of Chernobyl accident origin is developed. Розроблено розрахунково-експериментальний метод роздiлення сумарних α-активностей iзотопiв плутонiю A(²³⁹Pu+²⁴⁰Pu) на парцiальнi α-активностi A(²³⁹Pu) та А(²⁴⁰Pu) в аварiйних випаданнях Чорнобильського походження. Разработан расчетно-экспериментальный метод разделения суммарных α-активностей изотопов плутония A(²³⁹Pu+²⁴⁰Pu) на парциальные α-активности A(²³⁹Pu) и А(²⁴⁰Pu) в аварийных выпадениях Чернобыльского происхождения. This work was supported by the Ministry of Education and Sciences of Ukraine (grant No. M/68-2008) and the Byelorussian republican fund for fundamental researches (grant No. Φ09ΓKHT-003). en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Вопросы атомной науки и техники Ядернo-физические методы и обработка данных On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin О возможности разделения вкладов ²³⁹Pu та ²⁴⁰Pu в аварийных выпадениях плутония Чернобыльского происхождения О возможности разделения вкладов ²³⁹Pu та ²⁴⁰Pu в аварийных выпадениях плутония Чернобыльского происхождения Article published earlier |
| spellingShingle | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin Vodin, A.N. Olejnik, S.N. Rudak, E.A. Ushakov, I.V. Yachnik, O.I. Ядернo-физические методы и обработка данных |
| title | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin |
| title_alt | О возможности разделения вкладов ²³⁹Pu та ²⁴⁰Pu в аварийных выпадениях плутония Чернобыльского происхождения О возможности разделения вкладов ²³⁹Pu та ²⁴⁰Pu в аварийных выпадениях плутония Чернобыльского происхождения |
| title_full | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin |
| title_fullStr | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin |
| title_full_unstemmed | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin |
| title_short | On possibility of separation of ²³⁹Pu and ²⁴⁰Pu contributions in emergency plutonium fallout of Chernobyl accident origin |
| title_sort | on possibility of separation of ²³⁹pu and ²⁴⁰pu contributions in emergency plutonium fallout of chernobyl accident origin |
| topic | Ядернo-физические методы и обработка данных |
| topic_facet | Ядернo-физические методы и обработка данных |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/96513 |
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