Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium
The analysis of the properties of natural aluminosilicates in the conditions of various physical loadings and thermal factors are carred out. Microcline and clinoptilolite are inorganic materials having sorption opportunities to radionuclides. It is shown that under the effects of electrons, gamma q...
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України
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Dikiy, N.P. Bereznyak, O.P. Lyashko, Yu.V. Medvedeva, O.P. Medvedev, D.V. 2023-12-10T16:53:31Z 2023-12-10T16:53:31Z 2023 Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantum / N.P. Dikiy, O.P. Bereznyak, Yu.V. Lyashko, O.P. Medvedeva, D.V. Medvedev // Problems of Atomic Science and Technology. — 2023. — № 3. — С. 62-65. — Бібліогр.: 7 назв. — англ. 1562-6016 PACS: 89.30.Jj DOI: https://doi.org/10.46813/2023-145-062 https://nasplib.isofts.kiev.ua/handle/123456789/196141 The analysis of the properties of natural aluminosilicates in the conditions of various physical loadings and thermal factors are carred out. Microcline and clinoptilolite are inorganic materials having sorption opportunities to radionuclides. It is shown that under the effects of electrons, gamma quanta and thermal factors in natural aluminosilicates of various structures take place different radioaction stimulation of transformation which can be using for future perspective developments. Проведено аналіз властивостей природних алюмосилікатів в умовах дії різних фізичних навантажень та термальних факторів. Мікроклін та кліноптилоліт ‒ неорганічні матеріали, які мають сорбційні можливості до радіонуклідів. Показано, що під впливом електронів, гамма-квантів та термальних факторів у природних алюмосилікатах різної структури виникають різноманітні радіаційно-стимульовані трансформації, які можуть бути використані для майбутніх перспективних розробок. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Problems of Atomic Science and Technology Application of nuclear methods Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium Радіаційна стійкість природних алюмосилікатів різних структурних типів під впливом електронів та гамма-квантів Article published earlier |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| collection |
DSpace DC |
| title |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium |
| spellingShingle |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium Dikiy, N.P. Bereznyak, O.P. Lyashko, Yu.V. Medvedeva, O.P. Medvedev, D.V. Application of nuclear methods |
| title_short |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium |
| title_full |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium |
| title_fullStr |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium |
| title_full_unstemmed |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium |
| title_sort |
radiation stability of natural aluminosilicates various structural types by electrons and gamma quantium |
| author |
Dikiy, N.P. Bereznyak, O.P. Lyashko, Yu.V. Medvedeva, O.P. Medvedev, D.V. |
| author_facet |
Dikiy, N.P. Bereznyak, O.P. Lyashko, Yu.V. Medvedeva, O.P. Medvedev, D.V. |
| topic |
Application of nuclear methods |
| topic_facet |
Application of nuclear methods |
| publishDate |
2023 |
| language |
English |
| container_title |
Problems of Atomic Science and Technology |
| publisher |
Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| format |
Article |
| title_alt |
Радіаційна стійкість природних алюмосилікатів різних структурних типів під впливом електронів та гамма-квантів |
| description |
The analysis of the properties of natural aluminosilicates in the conditions of various physical loadings and thermal factors are carred out. Microcline and clinoptilolite are inorganic materials having sorption opportunities to radionuclides. It is shown that under the effects of electrons, gamma quanta and thermal factors in natural aluminosilicates of various structures take place different radioaction stimulation of transformation which can be using for future perspective developments.
Проведено аналіз властивостей природних алюмосилікатів в умовах дії різних фізичних навантажень та термальних факторів. Мікроклін та кліноптилоліт ‒ неорганічні матеріали, які мають сорбційні можливості до радіонуклідів. Показано, що під впливом електронів, гамма-квантів та термальних факторів у природних алюмосилікатах різної структури виникають різноманітні радіаційно-стимульовані трансформації, які можуть бути використані для майбутніх перспективних розробок.
|
| issn |
1562-6016 |
| url |
https://nasplib.isofts.kiev.ua/handle/123456789/196141 |
| citation_txt |
Radiation stability of natural aluminosilicates various structural types by electrons and gamma quantum / N.P. Dikiy, O.P. Bereznyak, Yu.V. Lyashko, O.P. Medvedeva, D.V. Medvedev // Problems of Atomic Science and Technology. — 2023. — № 3. — С. 62-65. — Бібліогр.: 7 назв. — англ. |
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2025-11-24T16:27:46Z |
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2025-11-24T16:27:46Z |
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| fulltext |
62 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145)
https://doi.org/10.46813/2023-145-062
RADIATION STABILITY OF NATURAL ALUMINOSILICATES
VARIOUS STRUCTURAL TYPES BY ELECTRONS AND
GAMMA QUANTIUM
N.P. Dikiy, O.P. Bereznyak, Yu.V. Lyashko, O.P. Medvedeva, D.V. Medvedev
National Science Center “Kharkov Institute of Physics and Technology”, Kharkiv, Ukraine
E-mail: ndikiy@kipt.kharkov.ua
The analysis of the properties of natural aluminosilicates in the conditions of various physical loadings and
thermal factors are carred out. Microcline and clinoptilolite are inorganic materials having sorption opportunities to
radionuclides. It is shown that under the effects of electrons, gamma quanta and thermal factors in natural
aluminosilicates of various structures take place different radioaction stimulation of transformation which can be
using for future perspective developments.
PACS: 89.30.Jj
INTRODUCTION
With deep disposal of radioactive waste, the
stability of the geological environment will be
determined mainly by its radioaction resistance and the
value of the absorbed dose of ionizing radioaction from
the radioactive waste located in it. To solve the
problem of safe isolation of radioactive waste, it is
necessary to evaluate the radioation resistance of
natural minerals depending on the mineral
composition, rock structure, selectivity, isomorphic
capacity, etc. in order to select the varieties of minerals
that are most resistant to radiaction exposure [1-5].
There are a sufficient number of publications on the
effect of irradiation on the structure of the natures of
minerals, but data on radiation-stimulated
transformations of the structure and phase composition
of rock-forming silicates that are part of the rocks of
radioactive waste, promising for the creation of
radioactive waste storages, are not enough.
The main rock-forming minerals of granitoid rocks
are aluminosilicates. The content of aluminosilicates is
~ 80%. The basis of the structure of silicates is a
silicon-oxygen tetrahedron, in the center of which there
is a silicon ion (Si
4+
), and at the peaks, there are
oxygen ions (O
2-
), which create tetravalent radicals
(SiO4)4.
The partial replacement of tetravalent silicon ions
by trivalent aluminum ions leads to the appearance of
an additional negative charge in the compound. Fig. 1
shows the microcline structure.
Fig. 1. Ordered microcline structure:
Al is located at one tetrahedral site (shaded),
Si is located at three other sites. Circles – location K
In this work, attention was paid to two minerals:
potassium feldspar ‒ microcline (K, Na)AlSi3O8, which
is the main rock-forming mineral that is part of
granitoids and clinoptilolite [(NaK)4CaAl6Si030O72
24H2O] ‒ high-siliceous natural zeolite [6].
The microcline studied in the work has an inclined
symmetry, but its crystal lattice can have a different
degree of deviation from monoclinic symmetry.
Fig. 2. The structure of clinoptilolite
A wide variety of properties of clinoptilolite is due
to its structural features Fig. 2. The crystalline
framework of clinoptilolite consists of [(Si,Al)O4]
octahedra combined into simple, double, and more
complex rings, has a sublayer structure, and a two-
dimensional system of channels. Since some of the Si
4+
ions are replaced by Al
3+
ions, this framework has a
negative charge, which is compensated by the presence
of Na
+
, K
+
, Ca
2+
, etc. cations. The total volume of
cavities and connecting channels filled with “zeolite
water” is ~ 50% of the crystal volume. The channel
diameter varies from 0.26 to 0.8 nm.
Similar crystal-chemical features of these minerals,
their ability to cation exchange, loss, and absorption of
water without destroying the structural framework,
allow us to consider them as natural matrix materials
and sorbets for long-term storage of radioactive waste
in Ukraine. In this regard, it is necessary to study the
resistance of these minerals to radiation exposure.
The purpose of this work was to determine the
features of the influence of radiation and thermal
factors on the properties of natural aluminosilicates
necessary for the safe immobilization of radionuclide.
mailto:ndikiy@kipt.kharkov.ua
ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145) 63
1. MATERIALS AND METHODS
The following objects were chosen as objects of
study: 1. white microcline fraction selected from
granitoids; 2. clinoptilolite of the Sokirnitskoe deposit
with a high SiO2 content (~70%) and the highest Si/Al
ratio ≥ 5.
The samples were irradiated on linear electron
accelerator with the following parameters: electron
energy Е ≈ 7 MeV, average beam current I = 500 µA,
temperature of the irradiated samples Т~ 40°С,
absorbed dose Dabs = 10
7
Gy at electron fluence
Ф = 3·10
16
…3·10
17
cm
-2
. The indicated dose range was
chosen because it is known that the maximum dose of
external radiation from radiofctive waste, that can be
collected by the geological enviroment for 1000 years,
is ~3.5·10
7
Gy. Irradiation of the samples was carried
out in sealed copper containers (copper foil thickness
0.5 mm) with water cooling.
Gamma-activation analysis was used to determine
the element content in the samples. The samples were
irradiated by bremsstrahlung from the linear
accelerator electron NSC KIPT with energy 23 MeV
and current 500 µA. Activation of samples was carried
out on air, the temperature of samples in the course of
activation did not exceed 40°C. Gamma activation
analyses is indestructible for native samples.
The determination of elements content in samples
performed by gamma-spectrometer method in Ge(Li) -
detector with the volume of 50 cm
3
and resolution of
3.2 at 1332 keV line. To reduce the influence of
background, the detector is equipped with a three-layer
Pb-Cu-Al protection. The errors of measurements were
from 7 to 25 %. The limit of detection elements for
photo activation analysis was 10
-4
…10
-7
wt.%.
Heat treatment of clinoptilolite was carried out at
260 and 750°C for 6 h to dehydrate and remove non-
zeolite components.
The structure and phase composition of samples
were investigation by infrared (IR) spectroscopy (IRS-
29, LOMO) in the frequency 400…4000 cm
-1
with a
measurement error of ± (2…7) cm
-1
. For IR
spectroscopy anlysis the samples were prepared in the
form of transparently compressed tablets from a
mixture of KBr and the test substance in an amount of
1% (100 mg sample). The pressing pressure was
9200 kg/cm
2
. To eliminate matrix absorptio bands, a
tablet of pure potassium bromide preliminarily dried at
180°C for 10 h was placed in the comparison channel
of the device. The powders were ground in agate
mortars to a size of ~1…10 μm and mixed in a special
closed box; pressing was carried out immediately
before the spectra were recorded. Graduation in the
range of 4000...700 cm
-1
was carried out according to
the spectrum of polystyrene with known frequencies of
absorption maxima, and in the range of 700…400 cm
-1
according to the bands of atmospheric water and CO2.
The correction averaged 15…5 cm
-1
.
Crystal optical studies were carried out on
polarizing microscope POLAM-L211 using immersion
liquides.
2. RESULTS AND DISCUSSION
Fig. 3 shows micrographs of grains of the initial
ordered microcline before and after irradiation to
D = 10
8
Gy. Without analyzer.
a
b
Fig. 3. Microphotographs of an immersion preparation
of initial microcline and after irradiation to
D=10
8
Gy, in transmitted light, view without an
analyzer. а – initial microcline; b – after irradiation to
D=10
8
Gy
The preparation of the initial microcline is
represented by pure grains with a characteristic lattice
structure with a small amount of secondary products of
pelitization up to 10% by volume.
Crystal optical studies of the microcline after
irradiation showed that with an increase in the
irradiation dose from 10
7
to 10
8
Gy, there is a gradual
decrease in the refractive index and a decrease in the
birefringence value to 0.003 (compared to the initial
0.008) due to the formation of secondary products of
pelitization and disorder of the crystal lattice.
The IR spectrum of the initial microcline (Fig. 4)
contains absorption maxima characteristic of this
mineral: a strong intensity band at 440 cm
-1
and a
group of bands in the region of 1040…1150 cm
-1
(Si-O
and Si-O-(Al) Si), as well as the bands of average
intensity 545, 595, 645, 735, 776 cm
-1
, characteristic
for the combined vibrations of Al-O-Si, Al-O, Si-O-Si
bonds.
The obtained γ-spectrum of activated clinoptilolite
revealed the presence of impurity radioactive isotopes
55
Fe,
54
Mn,
89
Zr,
237
U,
92m
Nb,
88
Y, etc., which have a
significant output of Auger electrons with energy from
2 to 6 keV from the reactions
56
Fe(γ,n)
55
Fe,
55
Mn(γ,n)
54
Mn (Fig. 5).
64 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145)
Fig. 4. IR spectra of 1 ‒ initial microcline; 2 ‒ after
irradiation to D=5∙10
7
Gy; 3 ‒ after irradiation to
D=10
8
Gy
Fig. 5. Gamma-spectrum of clinoptilolite
Having a high specific activity, Auger electrons can
form a significant number of electron-hole pairs (e-h
+
)
in a sample of clinoptilolite. Holes are able to split
water molecules in water-cationic subsystems, and
electrons that interact with dissolved oxygen molecules
generate highly reactive radicals such as singlet oxygen
(
1
O2), hydroxylic, etc., which, in turn, interact with H
+
and form radical HO2
-
and peroxides H2O2. The
presence of Fe in the “redox state” of aluminosilicates
increases the activation of the "Fenton reaction", which
is accompanied by the release of hydroxyl radicals
(OH
) and peroxide forms. A significant number of
highly reactive forms (oxygen atoms 10
19
…10
21
cm
-3
),
which were formed under the influence of ionizing
radiation, can form bonds with vacancies and
interassembliesl atoms, which creates conditions for
additional active centers that play a positive role in
sorption of radionuclides and immobilization of
radioactive waste.
Thus, -activation by bremsstrahlung on LAE on
porous aluminosilicates preserves chemical resistance
to leaching and stability of the crystal structure, but at
the same time realizes additional active centers of
sorption, which is the main high capacity.
Fig. 6. IR spectra of clinoptilolite samples
before (a) and after heat treatment at 260°(b)
and 700°C (c)
IR spectra of clinoptilolite samples before and after
heat treatment at 260 and 700°C are presented in Fig.
6. The spectrum of the initial sample (see Fig. 6, curve
a) is significantly different from the two almost
identical spectra of the samples after heat treatment
(curves b, c). In the IR spectrum of the initial sample,
the wide, smoothing contours of the bands,
characteristic of the water-saturated variety of
clinoptilolite, attract attention [6]. On the contrary, in
the spectra of heat-treated samples, intense absorption
bands of lattice vibrations of Si-O-Al tetrahedral
bonds, typical for crystalline monomineral zeolites, are
observed]. It can be noticed that the contour of each of
the wide bands in the spectrum of the original sample
almost completely corresponds to the total envelope for
the individual narrow bands of the series of frequencies
in the spectra of heat-treated samples.
A more detailed consideration in Fig. 6 spectra
show that the main bands relate to the valence bonds of
silicon and aluminum with oxygen and hydrogen with
oxygen. In the far IR region (ν ≤ 1150 cm
-1
), absorption
bands at 680, 740, and 1060…1120 cm
-1
associated
with lattice vibrations of external tetrahedral Si-O-Al
bonds are observed [7]. Along with this, the IR
spectrum contains bands at 1640…1650 and
3620…3440 cm
-1
, corresponding to vibrations of OH
bonds in zeolite water and hydroxyl groups ‒ Si-ON,
K-OH, Na-OH, Ca-(OH)
2
. In the region of 1340 cm
-1
, a
band corresponding to vibrations of Si-O bonds in
crystalline quartz appears. In the samples, there is also
an insignificant amount of amorphous silica – an
absorption band at 805 cm
-1
. In the region of
420…1150 cm
-1
, small maxima corresponding to
vibrations of Me-O bonds in oxides of impurity metals
(hematite, rutile, etc.) are observed.
Heat treatment at 260 and 700°C leads to
significant changes in the IR spectra of clinoptilolite,
indicating dehydration processes occurring in the
samples. However by the intensity of the band of
deformation vibrations of water (1645 cm
-1
), it can be
said that the main mass of molecularly sorbed water is
lost already after heat treatment at 260°C. However,
the intensity of this band decreases to zero only after
500 1000 1500
10
1
10
2
10
3
о
т
с
ч
е
ты
номер канала
208
Tl 583 keV
214
Bi 609keV
511 keV
228
Ac 911, 968 keV
40
K 1461 keV
214
Bi 1764 keV
212
Pb 238 keV
c
b
ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. №3(145) 65
holding the samples at 700°С. Additionally, both
spectra show a significant decrease in the intensity of
the bands associated with the valent vibrations of free
water in zeolites (3600 and 3440 cm
-1
) and the
absorption bands corresponding to the valent vibrations
of hydroxyl groups (3750…3450 cm
-1
).
Moreover, the absorption bands of hydroxyl groups
are observed after heat treatment at 260 and 700°С:
both spectra are characterized by a typical set of bands
‒ 3745, 3635, and 3580 cm
-1
. Hydroxyl groups,
corresponding to the absorption band at 3745 cm
-1
, can
be attributed to Si-ON groups, usually localized on
structural defects. This band is the weakest and is
observed in almost all spectra of natural zeolites,
regardless of the type of cations. On the contrary, the
intensity of absorption bands in the region of
3500…3600 cm
-1
depends on zeolites of cation
composition – the strong in the spectra of heylandite
and the weak in the spectra of clinoptilolite, which
corresponds to a decrease in the concentration of
divalent cations in clinoptilolite. In the context of this
fact, the noticeable decrease in the intensity of the
broad band in the interval 3650…3450 cm
-1
can be
explained mainly by the effect of the reduction of Ca-
(OH)2. Note that the Ca
2+
cation released from the
hydroxide, along with other cations (K
+
, Na
+
, etc.),
easily migrates and is incorporated into the structure of
clinoptilolite.
Changes in IR spectra in the region of
3750…3450 cm
-1
are especially clearly manifested in
the spectrum of the sample processed at 700°C (see
Fig. 6, curve c). It is possible to state that only
structural OH groups and their dehydroxylation
products are present in the sample after treatment at
700°С. Moreover, OH groups are groups formed
during dehydration, and not the original molecular
“zeolite” water. These groups are connected to the
framework of the zeolite and therefore are more heat-
resistant than the original crystalline hydrate water.
CONCLUSIONS
The study of changes in the structure and phase
composition of the main rock-forming aluminosilicates
under the influence of different types of irradiation
(electron and gamma quanta) showed: 1) as a result of
electron irradiation of the microcline, the formation of
structural defects and a gradual decrease in the cationic
orderliness occurs, which leads to the transition of the
microcline from an ordered to an intermediate state at
the maximum radiation dose up to D = 10
8
Gy. There is
also a decrease in the degree of triclinicity and the
disordering of the microcline due to the
monoclinization of the structure with the formation of
weakly crystallization products of secondary
pelitization; 2) a comparison of the radiation and
thermal effects on the structural-phase state of
clinoptilolite made it possible to establish the
unidirectional (towards a positive change) nature of
both processes.
These results are well comparable with numerous
new data on the high thermal and radiation stability of
aluminosilicates and on the possibility of using this
advantage for future promising developments.
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2. Radioactive waste disposal and geology. Top.Earth
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3. IAEA Safety Series. Safety Assessment for
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4. S. Masuda, H. Umeki, M. Natio. Reliability of High
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Article received 11.04.2023
РАДІАЦІЙНА СТІЙКІСТЬ ПРИРОДНИХ АЛЮМОСИЛІКАТІВ РІЗНИХ СТРУКТУРНИХ ТИПІВ
ПІД ВПЛИВОМ ЕЛЕКТРОНІВ ТА ГАММА-КВАНТІВ
М.П. Дикий, О.П. Березняк, Ю.В. Ляшко, О.П. Медведєва, Д.В. Медведєв
Проведено аналіз властивостей природних алюмосилікатів в умовах дії різних фізичних навантажень та
термальних факторів. Мікроклін та кліноптилоліт ‒ неорганічні матеріали, які мають сорбційні можливості до
радіонуклідів. Показано, що під впливом електронів, гамма-квантів та термальних факторів у природних
алюмосилікатах різної структури виникають різноманітні радіаційно-стимульовані трансформації, які можуть
бути використані для майбутніх перспективних розробок.
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