Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix
Nuclear reactions ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I were utilized for research of Cs and I diffusion in glassceramic matrices. The glassceramic matrix was manufactured with the help of hot isostatic pressing at 910°C and pressure 100 MPa. Diffusivities of cesium and iodine in a grain and through interp...
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України
2006
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| Cite this: | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix / N.P. Dikiy, S.V. Gabelkov, A.N. Dovbnya, Yu.V. Lyashko, E.P. Medvedeva, S.Yu. Saenko, A.E. Surkov, V.V. Tarasov, V.L. Uvarov, I.D. Fedorets, G.A. Holomeev, V.I. Borovlev, V.D. Zabolotny, D.V. Medvedev // Вопросы атомной науки и техники. — 2006. — № 3. — С. 171-173. — Бібліогр.: 6 назв. — англ. |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1859748247815323648 |
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| author | Dikiy, N.P. Gabelkov, S.V. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Saenko, S.Yu. Surkov, A.E. Tarasov, V.V. Uvarov, V.L. Fedorets, I.D. Holomeev, G.A. Borovlev, V.I. Zabolotny, V.D. Medvedev, D.V. |
| author_facet | Dikiy, N.P. Gabelkov, S.V. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Saenko, S.Yu. Surkov, A.E. Tarasov, V.V. Uvarov, V.L. Fedorets, I.D. Holomeev, G.A. Borovlev, V.I. Zabolotny, V.D. Medvedev, D.V. |
| citation_txt | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix / N.P. Dikiy, S.V. Gabelkov, A.N. Dovbnya, Yu.V. Lyashko, E.P. Medvedeva, S.Yu. Saenko, A.E. Surkov, V.V. Tarasov, V.L. Uvarov, I.D. Fedorets, G.A. Holomeev, V.I. Borovlev, V.D. Zabolotny, D.V. Medvedev // Вопросы атомной науки и техники. — 2006. — № 3. — С. 171-173. — Бібліогр.: 6 назв. — англ. |
| collection | DSpace DC |
| container_title | Вопросы атомной науки и техники |
| description | Nuclear reactions ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I were utilized for research of Cs and I diffusion in glassceramic matrices. The glassceramic matrix was manufactured with the help of hot isostatic pressing at 910°C and pressure 100 MPa. Diffusivities of cesium and iodine in a grain and through interphase boundary at 600°C were equal 10⁻¹¹ and 7.9⋅10⁻⁹ sm²/s, accordingly. The decrease of iodine diffusivity in a grain was observed at 750°C. A method of manufacture of glassceramic matrix for long-lived storage and nuclear-waste disposal ¹²⁹I is proposed.
Ядерные реакции ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I использовались для исследования диффузии Cs и I в стеклокерамической матрице. Стеклокерамическая матрица изготовлена при помощи газостатического прессования при 910°С и давлении 100 МПа. Коэффициенты диффузии цезия и йода в зерне и по границам зерен при 600°С составили 10⁻¹¹ и 7,9⋅10⁻⁹ см²/с, соответственно. Обнаружено уменьшение коэффициента диффузии йода в зерне при 750°С. Предложен способ создания матрицы для захоронения ¹²⁹I.
Ядерні реакції ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I використовувалися для дослідження дифузії Cs та I у склокерамічній матриці. Склокерамічна матриця виготовлена за допомогою газостатичного пресування при 910°С і тиску 100 МПа. Коефіцієнти дифузії цезію і йоду в зерні і по границях зерен при 600° С склали 10⁻¹¹ та 7,9⋅10⁻⁹ см²/с, відповідно. Виявлено зменшення коефіцієнта дифузії йоду в зерні при 750°С. Запропоновано спосіб створення матриці для поховання ¹²⁹I.
|
| first_indexed | 2025-12-01T22:48:35Z |
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APPLICATION OF GAMMA ACTIVATION ANALYSIS FOR RESEARCH
OF Cs AND I DIFFUSION INTO A GLASSCERAMIC MATRIX
N.P. Dikiy, S.V. Gabelkov, A.N. Dovbnya, Yu.V. Lyashko, E.P. Medvedeva, S.Yu. Saen-
ko, A.E. Surkov, V.V. Tarasov, V.L. Uvarov, I.D. Fedorets1, G.A. Holomeev, V.I. Borovlev,
V.D. Zabolotny, D.V. Medvedev
NSC KIPT, Kharkiv, Ukraine,
1V.N. Karazin KрNU, Kharkiv, Ukraine
E-mail: ndikiy@kipt.kharkov.ua
Nuclear reactions 133Cs(γ,n)132Cs, 127I(γ,n)126I were utilized for research of Cs and I diffusion in glassceramic ma-
trices. The glassceramic matrix was manufactured with the help of hot isostatic pressing at 910°C and pressure
100 MPa. Diffusivities of cesium and iodine in a grain and through interphase boundary at 600°C were equal 10−11
and 7.9⋅10−9 sm2/s, accordingly. The decrease of iodine diffusivity in a grain was observed at 750°C. A method of
manufacture of glassceramic matrix for long-lived storage and nuclear-waste disposal 129I is proposed.
PACS: 29.17.+w, 28.41Kw
INTRODUCTION
The multibarrier protection of the biosphere against
radionuclides [1] for nuclear-waste disposal and long-
term storage of high-level waste (HLW) is carried out
by means of: 1) a stable matrix, retaining radionuclides;
2) a multilayer engineering barrier; 3) a geologic medi-
um of nuclear-waste disposal.
The geologic medium is a basic barrier for radionu-
clide diffusion at the time of the nuclear-waste disposal
or long-term storage of high-level waste. The synthetic
engineering barriers execute protective functions mainly
during the period before the final conservation of a
storehouse and during the initial period of a geologic
storage. In the case of a temporal surface or near-surface
storage of HLW, the basic load on isolation of the ra-
dioactive waste is realized by means of the engineer
barrier.
The borosilicate glass has been considered as a ref-
erence industrial matrix for conditioning solutions of
fission products (comprising more than thirty chemical
elements) resulting from spent-fuel reprocessing opera-
tions.
Swelling clays can be used in the engineered barrier
system of geologic repositories. Swelling clays placed
between the excavated rock and the waste containers in
a repository can mechanically fill the open volume,
buffer the chemistry around container, and retard ra-
dionuclides migration.
The engineering barrier can be improved by means
of a spent fuel immobilization. One of perspective
methods of the HLW immobilization is to build the bar-
riers made of glassceramic matrix. For prediction mass
transfer in the HLW immobilisation during the nuclear-
waste disposal, it is necessary to define their diffusive
constants. Studies into a joint diffusion of elements with
sharply distinguished properties (for example, alkaline
and halogens elements) are in particular interest.
EXPERIMENTAL SET-UP AND METHODS
In the present article the diffusion of Cs and I in the
glassceramic matrix (70% of granite +30% of kaolin),
manufactured by means of hot isostatic pressing (HIP)
was investigated. The HIP-handling was carried out at
920°С and 100 МPa during 5 hours.
The glassceramic material is characterized by high
density (relative density more than 0.99). It has satisfac-
tory mechanical fastness, high corrosion stability, and
radiation stability and can be applied as a material of the
barrier layer for capsulation of the radioactive waste and
HLW.
On a polished surface of the glassceramic sample the
CsI tracer stratum was coated. The tracer exposed to a
short-term heating within 10…15 minutes in gasostat
for embodying contact with the sample. The diffusion
was carried out in air during 300 hours at Т=600°C and
750°С [2]. The samples were irradiated by
bremsstrahlung radiation of an electron accelerator with
energy 23 MeV during 3 days after removal of CsI
tracer. The penetration profiles of Cs and I were meas-
ured by the method of removal layers. The activity of
the stratums removed was measured with a Ge(Li)-de-
tector by registering the isotope radiation with energy
668 keV and 388 keV from the reactions 133Cs(γ,n)132Cs,
127I(γ,n)126I.
RESULTS AND DISCUSSION
The obtained profiles of Cs and I are shown in
Fig.1, 2. The full curves are obtained (for Cs and I at
Т = 600°С, for Cs at Т = 750°С) using the least-squares
procedure for the diffusion expression [3, 4]. The char-
acteristic dependence of Cs and I isotopes’ densities
versus the sample depth is observed. The Cs diffusion
realize in a grain (0…120 µm for Т=600°С, 0…250 µm
for Т=750°С) and in crystal boundaries (more 250 µm).
Calculation of diffusion element in the matrix is car-
ried out by the expression [4]:
____________________________________________________________
PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2006. № 3.
Series: Nuclear Physics Investigations (47), p.171-173. 171
( )
( ){ }XerfcXXe
d
b
tmaD
erfc
C
yС
∗∗−
−
−∫
∞
×
×+=
−
π
σ
η
σ
σ
π
ηη
2
4
2
exp
1 2/3
20 (1)
X = (σ−1)/2⋅β, Dma=Dm/(1+ρm⋅Kd/εm), (2)
Dfa=Dfa/(εm+ρmKd), (3)
tmaD
y
=η ,
tmaD
∆
=β ,
maD
faaD
=∆ , (4)
where a is a half-width of a fissure, b – a half-interval,
Co– initial tracer concentration of solution, Df – fissure
diffusion coefficient, Dfa – fissure apparent diffusion co-
efficient, Dma – apparent diffusion coefficient in pore
water of matrix, Kd – adsorption coefficient, εm – the
matrix porosity, ρm – the matrix density, y - distance
from the specimen surface in the direction of depth.
The first term on the right-hand side of the eq.(1)
represents the direct diffusion into grains and is a func-
tion of y only. The second term represents the contribu-
tion of the diffusion through the fissure.
Diffusion coefficient is determined by means of
minimization function [5]:
F=(Σ(yth-yexp)2/(k-s), (5)
where yth, yexp − theoretical and experimental values the
reaction yield, accordingly, k – the measurements’ num-
ber, s – the number of connections (number of degrees
of distribution). The minimal function values were real-
ized at b=50 µm (radius of the grain).
The Cs and I diffusivities in the grains and through
grain borders are equal to 10−11 and 7.9⋅10−9 sm2/s at
Т=600°С, accordingly. An essential difference in the io-
dine profiles is visible at Т=600°C and 750°С. At
Т=750°С the maximal iodine density value is observed
at 200 µm. For Cs at the same temperature the smooth
lowering of the density is observed.
It is known that due to the Coulomb attraction a
polyvalent cation together with cationic vacancy forms
a complex cluster «admixture−cationic vacancy». At
presence of such complexes the diffusivities of the
cations D+ and anions D− are equal [6]:
D+ = 4⋅a2⋅f⋅νo⋅exp((Sm+)/k)⋅exp((−Hm+)/k⋅T), (6)
D− = (4⋅a2⋅f⋅νo⋅/c)⋅exp((Sm−)/k)⋅exp((−Hm−)/k⋅T), (7)
where νo is the effective vibration frequency of an ion
being near the equilibrium position (is supposed identi-
cal to the anionic and cationic vacancies), f - the corre-
lation factor, and a - distance between the anion and
cation, c - isovalent atom density, Sm+, Hm+ - entropy and
enthalpy of migration of the cations, Sm−, Hm− - entropy
and enthalpy of migration of the anions, k - the Boltz-
mann constant, Т - temperature. It is apparent that the
anion diffusivity is inversely proportional to the isova-
lent atom density.
Generally, the glassceramics obtained consists of
feldspar (Na2O⋅Al2O3⋅6SiO2), mullite (2SiO2⋅3Al2O3),
glass, and other minerals and is characterized by the
presence of the cations of different valence. The expres-
sions 6, 7 adjusted describe the cation self-diffusion in a
lattice such as NaCl at presence of isovalent admixtures.
Therefore, in our case, these expressions can serve as
estimation.
Note, the cations c+ and c− density agreed with Lida-
jrd [6] is:
с+⋅с− = exp(−Gs/k⋅T), (8)
where Gs is Gibbs free energy of the Schottky couple
formation. Therefore, the cesium diffusion increases and
iodine diffusion decreases over a period of time.
This fact exhibits the different character of these ele-
ments concentration dependence (Fig.1,2). The cation
diffusion increases, whereas anion diffusion decreases
for the cation density less than 10-2% (see, [3]).
0 100 200 300 400
0,1
1
10
0 2 4 6 8 10
0
2
4
6
8
10
co
nt
en
t,
m
g/
g
depth, µ m
I, 600oC
Cs, 600oC
Fig.1. Penetration profiles of I and Cs in a glassceram-
ic after diffusion during 300 hours at 600°С
0 100 200 300 400 500 600 700
10
100
0 2 4 6 8 10
0
2
4
6
8
10
co
nt
en
t,
m
g/
g
depth, µ m
I 750oC
Cs 750oC
Fig.2. Penetration profiles of I and Cs in a glassceram-
ic after diffusion during 300 hours at 750°С
172
It should be noted that the frequency factor change
for Cs+ (atomic radius 1.69 Å) in comparison with other
alkaline ions is more significant, than for I+ (atomic ra-
dius 2.16 Å) in comparison with other halogens.
The absence of inconvertible natural minerals con-
taining I at an age of about 108 years causes the problem
of matrix synthesis the nuclear-waste disposal of 129I.
Apparently, our results obtained and presented here can
be used in manufacturing of a prime glassceramic ma-
trix with considerable density of 129I (0.3% mass.). Sta-
bilization of 129I is realized by the alkaline elements.
The work is supported by the project X866 of the
program NMRT2010.
REFERENCES
1. O.K. Avdeev, A.A. Kretinin, A.I. Ledenev et al. Ra-
dioactive waste of Ukraine: State, problem, solution.
Kiev: DrUk, 2003 (in Russian).
2. N.P. Dikiy, V.P. Kantsedal, I.M. Neklydov et al.
Researches and technological developments of new
ceramic compositions for an immobilization of a ra-
dioactive wastage // Problems of Atomic Science
and Technology. Series: Nuclear Physics Investiga-
tions. 2002, №2(40), p.25-39.
3. I.Kaur, W. Gust. Fundamentals of grain and inter-
phase boundary diffusion. Stuttgard: “Zigler Press”,
1989.
4. K. Idemitsu, H. Furuya et al. Primary Diffusion
Path of Uranium (VI) in Laboratory Scale Water-
saturated Inada Granite. Proc. of Inter. Conf. on
Nuclear Waste Management and Environmental
Remediation. 1993, v.1, p.207-212.
5. N.P. Dikiy. Nuclear physics technique for adjacent
regions // Problems of Atomic Science and Tech-
nology. Series: Nuclear Physics Investigations.
2003, №2(41), p.25-29.
6. A.Lidajrd. Ion conductance of crystals. M.:”IL”,
1962 (in Russian).
ПРИМЕНЕНИЕ ГАММА-АКТИВАЦИОННОГО АНАЛИЗА ДЛЯ ИССЛЕДОВАНИЯ
ДИФФУЗИИ Cs И I В СТЕКЛОКЕРАМИЧЕСКОЙ МАТРИЦЕ
Н.П. Дикий, С.В. Габелков, А.Н. Довбня, Ю.В. Ляшко, Е.П. Медведева, С.Ю. Саенко, А.Е. Сурков,
В.В. Тарасов, В.Л. Уваров, И.Д. Федорец, Г.А. Холомеев, В.И. Боровлев, В.Д. Заболотный, Д.В. Медведев
Ядерные реакции 133Cs(γ,n)132Cs, 127I(γ,n)126I использовались для исследования диффузии Cs и I в стеклоке-
рамической матрице. Стеклокерамическая матрица изготовлена при помощи газостатического прессования
при 910°С и давлении 100 МПа. Коэффициенты диффузии цезия и йода в зерне и по границам зерен при
600°С составили 10−11 и 7,9⋅10−9 см2/с, соответственно. Обнаружено уменьшение коэффициента диффузии
йода в зерне при 750°С. Предложен способ создания матрицы для захоронения 129I.
ЗАСТОСУВАННЯ ГАММА-АКТИВАЦІЙНОГО АНАЛІЗУ ДЛЯ ДОСЛІДЖЕННЯ ДИФУЗІЇ Cs ТА I
В СКЛОКЕРАМІЧНІЙ МАТРИЦІ
М.П. Дикий, С.В. Габелков, А.М. Довбня, Ю.В. Ляшко, Е.П. Медведєва, С.Ю. Саєнко, А.Е. Сурков,
В.В. Тарасов, В.Л. Уваров, І.Д. Федорець, Г.А. Холомеєв, В.І. Боровльов, В.Д. Заболотний, Д.В. Медведєв
Ядерні реакції 133Cs(γ,n)132Cs, 127I(γ,n)126I використовувалися для дослідження дифузії Cs та I у
склокерамічній матриці. Склокерамічна матриця виготовлена за допомогою газостатичного пресування при
910°С і тиску 100 МПа. Коефіцієнти дифузії цезію і йоду в зерні і по границях зерен при 600°С склали 10−11
та 7,9⋅10−9 см2/с, відповідно. Виявлено зменшення коефіцієнта дифузії йоду в зерні при 750°С.
Запропоновано спосіб створення матриці для поховання 129I.
____________________________________________________________
PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2006. № 3.
Series: Nuclear Physics Investigations (47), p.171-173. 173
INTRODUCTION
RESULTS AND DISCUSSION
REFERENCES
|
| id | nasplib_isofts_kiev_ua-123456789-79882 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-01T22:48:35Z |
| publishDate | 2006 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Dikiy, N.P. Gabelkov, S.V. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Saenko, S.Yu. Surkov, A.E. Tarasov, V.V. Uvarov, V.L. Fedorets, I.D. Holomeev, G.A. Borovlev, V.I. Zabolotny, V.D. Medvedev, D.V. 2015-04-06T15:35:26Z 2015-04-06T15:35:26Z 2006 Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix / N.P. Dikiy, S.V. Gabelkov, A.N. Dovbnya, Yu.V. Lyashko, E.P. Medvedeva, S.Yu. Saenko, A.E. Surkov, V.V. Tarasov, V.L. Uvarov, I.D. Fedorets, G.A. Holomeev, V.I. Borovlev, V.D. Zabolotny, D.V. Medvedev // Вопросы атомной науки и техники. — 2006. — № 3. — С. 171-173. — Бібліогр.: 6 назв. — англ. 1562-6016 PACS: 29.17.+w, 28.41Kw https://nasplib.isofts.kiev.ua/handle/123456789/79882 Nuclear reactions ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I were utilized for research of Cs and I diffusion in glassceramic matrices. The glassceramic matrix was manufactured with the help of hot isostatic pressing at 910°C and pressure 100 MPa. Diffusivities of cesium and iodine in a grain and through interphase boundary at 600°C were equal 10⁻¹¹ and 7.9⋅10⁻⁹ sm²/s, accordingly. The decrease of iodine diffusivity in a grain was observed at 750°C. A method of manufacture of glassceramic matrix for long-lived storage and nuclear-waste disposal ¹²⁹I is proposed. Ядерные реакции ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I использовались для исследования диффузии Cs и I в стеклокерамической матрице. Стеклокерамическая матрица изготовлена при помощи газостатического прессования при 910°С и давлении 100 МПа. Коэффициенты диффузии цезия и йода в зерне и по границам зерен при 600°С составили 10⁻¹¹ и 7,9⋅10⁻⁹ см²/с, соответственно. Обнаружено уменьшение коэффициента диффузии йода в зерне при 750°С. Предложен способ создания матрицы для захоронения ¹²⁹I. Ядерні реакції ¹³³Cs(γ,n)¹³²Cs, ¹²⁷I(γ,n)¹²⁶I використовувалися для дослідження дифузії Cs та I у склокерамічній матриці. Склокерамічна матриця виготовлена за допомогою газостатичного пресування при 910°С і тиску 100 МПа. Коефіцієнти дифузії цезію і йоду в зерні і по границях зерен при 600° С склали 10⁻¹¹ та 7,9⋅10⁻⁹ см²/с, відповідно. Виявлено зменшення коефіцієнта дифузії йоду в зерні при 750°С. Запропоновано спосіб створення матриці для поховання ¹²⁹I. The work is supported by the project X866 of the program NMRT2010. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Вопросы атомной науки и техники Применение ускорителей в радиационных технологиях Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix Применение гамма-активационного анализа для исследования диффузии Cs и I в стеклокерамической матрице Застосування гамма-активаційного аналізу для дослідження дифузії Cs та I в склокерамічній матриці Article published earlier |
| spellingShingle | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix Dikiy, N.P. Gabelkov, S.V. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Saenko, S.Yu. Surkov, A.E. Tarasov, V.V. Uvarov, V.L. Fedorets, I.D. Holomeev, G.A. Borovlev, V.I. Zabolotny, V.D. Medvedev, D.V. Применение ускорителей в радиационных технологиях |
| title | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix |
| title_alt | Применение гамма-активационного анализа для исследования диффузии Cs и I в стеклокерамической матрице Застосування гамма-активаційного аналізу для дослідження дифузії Cs та I в склокерамічній матриці |
| title_full | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix |
| title_fullStr | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix |
| title_full_unstemmed | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix |
| title_short | Application of gamma activation analysis for research of Cs and I diffusion into a glassceramic matrix |
| title_sort | application of gamma activation analysis for research of cs and i diffusion into a glassceramic matrix |
| topic | Применение ускорителей в радиационных технологиях |
| topic_facet | Применение ускорителей в радиационных технологиях |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/79882 |
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