Investigation of granite rocks radiation-chemical durability
Gamma-activation analysis is used to study dynamics of leaching of various elements from granite samples. The sample preliminary irradiation and activation was carried out in the field of bremsstrahlung of electron accelerator. With the use of Ge(li) detector concentration of sodium, cesium and mang...
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| Опубліковано в: : | Вопросы атомной науки и техники |
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| Дата: | 2002 |
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України
2002
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| Цитувати: | Investigation of granite rocks radiation-chemical durability / Investigation of granite rocks radiation-chemical durability // Вопросы атомной науки и техники. — 2002. — № 2. — С. 61-63. — Бібліогр.: 15 назв. — англ. |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1859913094725107712 |
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| author | Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Sayenko, S.Yu. Tarasov, R.V. Uvarov, V.L. Kholomeyev, G.A. Shevyakova, E.P. Fedorets, I.D. |
| author_facet | Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Sayenko, S.Yu. Tarasov, R.V. Uvarov, V.L. Kholomeyev, G.A. Shevyakova, E.P. Fedorets, I.D. |
| citation_txt | Investigation of granite rocks radiation-chemical durability / Investigation of granite rocks radiation-chemical durability // Вопросы атомной науки и техники. — 2002. — № 2. — С. 61-63. — Бібліогр.: 15 назв. — англ. |
| collection | DSpace DC |
| container_title | Вопросы атомной науки и техники |
| description | Gamma-activation analysis is used to study dynamics of leaching of various elements from granite samples. The sample preliminary irradiation and activation was carried out in the field of bremsstrahlung of electron accelerator. With the use of Ge(li) detector concentration of sodium, cesium and manganese isotopes in the leachant as well as the dependence of diffusion coefficient are determined.
|
| first_indexed | 2025-12-07T16:03:08Z |
| format | Article |
| fulltext |
INVESTIGATION OF GRANITE ROCKS RADIATION-CHEMICAL
DURABILITY
N.P. Dikiy, A.N. Dovbnya, Yu.V. Lyashko, E.P. Medvedeva, S.Yu. Sayenko, R.V. Tarasov
V.L. Uvarov, G.A. Kholomeyev, E.P. Shevyakova, I.D. Fedorets1
National Science Center “Kharkov Institute of Physics and Technology”, Kharkov, Ukraine
e-mail: sayenko@kipt.kharkov.ua
1Kharkov National University, Kharkov, Ukraine
Gamma-activation analysis is used to study dynamics of leaching of various elements from granite samples. The
sample preliminary irradiation and activation was carried out in the field of bremsstrahlung of electron accelerator.
With the use of Ge(li) detector concentration of sodium, cesium and manganese isotopes in the leachant as well as
the dependence of diffusion coefficient are determined.
PACS: 07.85.-Nc, 07.88.+y, 81.70-q, 93.00.00
1. INTRODUCTION
Managing spent nuclear fuel supposes it to be kept in
water pools and dry storage facilities at the nuclear
plants for 10-50 years with the following placing in the
geological repositories. During disposal in the
geological structures the long-living isotopes of nuclear
fuel fission has particular importance: 99Tc (period of
half-decay T1/2 makes up to 2,1⋅105 years),
129I (T1/2 = 1,6⋅107 y), 135Cs (T1/2 = 2,3⋅106 y), 93Zr (T1/2 =
1,5⋅106y), 126Sn (T1/2 = 105 y), 79Se (T1/2 = 6,5⋅104 y),
137Cs (T1/2= 30,2 y), 90Sr (T1/2= 28 y) and actinides:
239Pu (T1/2 = 2,4⋅104 y), 240Pu (T1/2 = 6,5⋅103 y),
242Pu(T1/2 = 3,8⋅105 y), 241Am (T1/2= 432 y), 244Cm(T1/2 =
18 y). The most ecologically dangerous from these
elements are 137Cs, 135Cs, 129I, 99Тс. They are dissolved in
the water and can easily get into the biological cycle.
From the total amount of materials intended for disposal,
the volume containing these elements is up to 90% [1].
In Ukraine, the repositories for long-term disposal of
radioactive wastes (RAW) are supposed to place in
geological structures of the Ukrainian Crystalline Shield
(UCS) [2]. Therefore, the investigation of durability of
UCS rocks as a geological barrier under the condition of
radiation effect is a topical problem. It is also stipulated
by the possibility to use the component of the UCS
rocks to immobilize RAW. Of particular interest is the
study of long-living radionuclides migration during
corrosion processes in the mountain rocks.
Applying nuclear-physical methods is rather an
efficient means to research radionuclides diffusion and
leaching processes [3-6].
The purpose of the work was developing the method
of researching the diffusion processes of leaching
materials and Mn (Tc analogue in chemical properties)
in non-organic materials under the terms of the
combined (radiation and corrosion) effect as well as
demonstrating the possibilities of this method on the
example of the granite samples.
2. THE METHODS OF EXPERIMENT
For the investigation granite samples of UCS
Dneprovskiy deposit made in the shape of
parallelepiped with the size 10x10x10.5 mm and mass
(2,8-2,9) g were chosen. The samples were irradiated in
the field of bremsstrahlung of the electron accelerators
at two stages: first – at the value of upper boundary of
the photon energetic spectrum Eγ max=10 MeV up to the
value of the absorbed dose (AD) 1,7⋅107 Gy, after that
the samples were activated at Eγ max=23 MeV during 7
days up to the summary value of AD 3,0⋅107 Gy. Then
the samples were kept for some days to reduce the level
of the induced radioactivity, ground up into granules
with the size less than 0.83 mm which allowed to
increase their surface area from 6,2 to 59 cm2 and
underwent dynamic tests on leaching in the plant based
on Soxhlet extractor [7] by methods described in work [8].
Soxlet extractor is traditionally used in geological
research to carry out prolonged experiments simulating
the process of natural weathering.
The temperature of the leachant in the cylinder of the
extractor was 72°C. The leachant was discharged every
1,5, 3,5, 30, 105 and 113 hours. After each discharge of
the leachant its activity was measured by Ge(Li)
spectrometer with power identification 2,8 keV (on the
line Eγ=1333 keV). This approach made it possible to
study dynamics of leaching the various chemical
elements from the investigated samples with high
sensitivity.
3. EXPERIMENTAL RESULTS AND
DISCUSSION
3.1. Gamma-activation analysis of samples showed
that the feature of the element composition of the
studied granite is the increased content of uranium –
10 µg/g 3 times exceeding its characteristics clark value.
The content of Zr and Nb in the sample was also higher
than characteristic values.
PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2002, № 2.
Series: Nuclear Physics Investigations (40), p. 61-63. 61
The typical spectrum of gamma-radiation of the
granite sample after activation is given on Fig.1. On the
spectrum the lines from photo-nuclear reaction on the
matrix and microelements of granite can be definitely
see: 48Ca(γ,n)47Ca→47Sc, 23Na(γ,n)22Na, 23Na(n,γ)24Na,
93Nb(γ,n)92mNb, 85Rb(γ,n)84Rb, 89Y(γ,n)88Y, 133Cs(γ
,n)132Cs, 55Mn(γ,n)54Mn, 238U(γ,n)237U. The element and
crystal-optic analysis of the samples allowed defining
the granite composition (see the table).
1
10
100
1000
Co
un
ts
511
1369
Na
1275
Na
1297
Ca
835
Mn
1078
Rb
935
Nb
909
Zr881
Rb
208
U
668
Cs
159
Sc
0 400 800 1200 1600 2000
Channel
47
237
132
84
54
898
Y88
89
92m
86
22
47
24
Energy of gamma-qauntums, keV
Fig. 1. γ-spectrum of granite sample after activating by
bremsstrahlung
Chemical and mineralogical compositions
Chemical
composition Mineralogical composition
Oxide %, mas Mineral %,mas
SiO2 72,9 Quartz (SiO2) 25-30
Al2O3 14,1
Fe2O3
FeO 2,2
Potassium feldspars
(orthoclase, microcline)
K(Na)AlSi3O8
55-60
CaO 1,4 Acid plagioclases, albite
Na(Ca)AlSi3O8
<10
MgO 1,0
K2O,
Na2O
8,4
Color mica, biotite
K(Mg,Fe,Mn)3⋅
[AlSi3O10(OH,F)2]
10-12
Muscovite
2[K2Аl4(Si6Al2O20)(OH,F)4]
<1
TiO2 < 0,1 Accessory: garnet, zircon,
apatite, monazite and ore
minerals: magnetite, hematite
<1
3.2. The leachant spectrum after 113 hours of
leaching is showed on Fig.2. Its analysis shows that
sodium, rubidium and calcium are leached from granite
most intensely. There was no noticeable release of
uranium and yttrium from this sample.
3.3. Amount q of substance of passed through the
unity of the sample surface for time t, in our case can be
expressed like that [9]:
q = (2/π1/2) co (Dt)1/2, (1)
where C0 – concentration of the element under
investigation in the granite sample, D – coefficient of
diffusion of this element in the sample. Using the values
of stream densities (rates of leaching) Na, Rb, Cs and
Mn obtained during the experiment, their coefficients of
diffusion were calculated from the equation (1).
Dependencies of diffusion coefficients of these elements
on the logarithm of the leaching time are given on
Fig. 3.
0 4 0 0 8 0 0 1 2 0 0 1 6 0 0 2 0 0 0
Channel
1
1 0
1 0 0
C
ou
nt
s
1 5 9
S c
5 1 1
1 4 6 1
K
1 2 7 5
N a
8 3 5
M n 8 8 1
R b
Energy of gamma-quantums, keV
4 7
5 4
8 4
2 2 4 0
Fig. 2. γ-spectrum of leachant
3,0 3,5 4,0 4,5 5,0 5,5 6,0
1E-16
1E-15
1E-14
1E-13
1E-12
D
, с
м2 /c
lg(t)
Rb
Na
Cs
Mn
Fig. 3. Coefficients of diffusion of alkaline elements
and Mn
3.4. As it follows from the data obtained,
coefficients of diffusion Na and Rb reduce depending on
the time of leaching while coefficient of diffusion Cs in
the studied interval of time remains the constant value.
Coefficient of diffusion Mn increases considerably
which might be stipulated by forming the hydro oxides
layer on the surface [10-12]. The fact that Mn is similar
to 99Tc in chemical properties is significant during
choosing the places for RAW long-term disposal in
geological structures.
It is noteworthy that coefficient of diffusion Na are
the lowest. Higher values are observed for Rb and the
highest for Cs. Ion radii Na, Rb, Cs and K make up
0,098; 0,149; 0,165 and 0,133 nm correspondingly.
Potassium feldspars and plagioclase amount 65-70% of
mass in the granite under study. Rb and Cs being a part
of them have bigger ion radii as compared to potassium
thus causing due to elastic deformation g the crystalline
lattice the essential change of pre-experimental
(frequency) factor D0 in the expression for coefficient of
diffusion D:
D=D0exp(-Q/RT), (2)
62
where Q – energy of activation, R – gas constant, T –
absolute temperature.
D0 is stipulated by physico-chemical properties of
the crystal. In the first approximation the noticeable
change of the frequency of atom fluctuation ω:
ω = (1/π)(K/M)1/2, (3)
where M – mass of isotope, K – coefficient of the elastic
increasing force for particle moving in the potential well
V(x)=V(x0)+0,5K(x-x0)2. As calculation shows [13] the
frequency factor for Cs is 5 times as high as for Na in
NaCl. Isomorphous substitution of a certain part of
potassium by sodium in the potassium feldspars does not
cause deformation of the crystalline latter, sodium being
included in plagioclase as mineral forming component.
Therefore coefficients of diffusion Na have minimum
values.
Coefficients of diffusion of leaching metals and
manganese in granite samples of UCS, which are not
irradiated, are 30% less relative to the irradiated
ones [10,14,15].
CONCLUSIONS
1. There has been developed the method of
investigation of the radiation and chemical stability of
non-organic materials that can be used for choosing
perspective environments for deep geological disposal
of the radioactive wastes. The method includes dynamic
tests on leaching the samples of materials which
underwent the combined irradiation in the field of
bremsstrahlung of the electron accelerator with the
following analysis samples gamma-irradiation and
leachant. Sensitivity of the method is by factor of value
higher than that of the traditionally used chemical
methods of the leachant analysis.
2. Possibilities of the granite of Dneprovskiy deposit
of the Ukrainian Crystalline Shield. The obtained
coefficients of diffusion Na, Rb and Cs depending on
the time of leaching allow to prognose durability of the
granite as a geological barrier relative to the release of
radionuclides under the condition of radiation and
corrosion effect.
3. Behaviour of Mn in the system granite-water
under these conditions requires further specification and
studying.
ACKNOWLEDGMENTS
The work is carried out with the support of the
Science and Technology Center in Ukraine in the
framework of the project №1580.
The authors are grateful to Professor V.I. Zmiy for a
technical review of the paper and Mr A.E. Surkov for
help in formatting the text.
REFERENCES
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captures for element activation and waste
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gation of possibility to dispose radioactive wastes
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3. N.P. Dikiy, S.Yu. Sayenko, V.L. Uvarov,
E.P. Shevyakova. Application of nuclear-physics
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63
1Kharkov National University, Kharkov, Ukraine
PACS: 07.85.-Nc, 07.88.+y, 81.70-q, 93.00.00
Chemical and mineralogical compositions
CONCLUSIONS
ACKNOWLEDGMENTS
REFERENCES
|
| id | nasplib_isofts_kiev_ua-123456789-80116 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-07T16:03:08Z |
| publishDate | 2002 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Sayenko, S.Yu. Tarasov, R.V. Uvarov, V.L. Kholomeyev, G.A. Shevyakova, E.P. Fedorets, I.D. 2015-04-12T06:19:21Z 2015-04-12T06:19:21Z 2002 Investigation of granite rocks radiation-chemical durability / Investigation of granite rocks radiation-chemical durability // Вопросы атомной науки и техники. — 2002. — № 2. — С. 61-63. — Бібліогр.: 15 назв. — англ. 1562-6016 PACS: 07.85.-Nc, 07.88.+y, 81.70-q, 93.00.00 https://nasplib.isofts.kiev.ua/handle/123456789/80116 Gamma-activation analysis is used to study dynamics of leaching of various elements from granite samples. The sample preliminary irradiation and activation was carried out in the field of bremsstrahlung of electron accelerator. With the use of Ge(li) detector concentration of sodium, cesium and manganese isotopes in the leachant as well as the dependence of diffusion coefficient are determined. The work is carried out with the support of the Science and Technology Center in Ukraine in the framework of the project №1580. The authors are grateful to Professor V.I. Zmiy for a technical review of the paper and Mr A.E. Surkov for help in formatting the text. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Вопросы атомной науки и техники Application of the nuclear methods Investigation of granite rocks radiation-chemical durability Исследование радиационно-химической устойчивости гранитных пород Article published earlier |
| spellingShingle | Investigation of granite rocks radiation-chemical durability Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Medvedeva, E.P. Sayenko, S.Yu. Tarasov, R.V. Uvarov, V.L. Kholomeyev, G.A. Shevyakova, E.P. Fedorets, I.D. Application of the nuclear methods |
| title | Investigation of granite rocks radiation-chemical durability |
| title_alt | Исследование радиационно-химической устойчивости гранитных пород |
| title_full | Investigation of granite rocks radiation-chemical durability |
| title_fullStr | Investigation of granite rocks radiation-chemical durability |
| title_full_unstemmed | Investigation of granite rocks radiation-chemical durability |
| title_short | Investigation of granite rocks radiation-chemical durability |
| title_sort | investigation of granite rocks radiation-chemical durability |
| topic | Application of the nuclear methods |
| topic_facet | Application of the nuclear methods |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/80116 |
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