Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste
In this review, the issues of radiation and nucleus safety at dealing with nuclear waste (RW) are considered. The examples of already worked out technologies on definition of the isotopes contents of uranium and plutonium in radioactive waste are adduced; the possibilities of implementation of techn...
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України
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nasplib_isofts_kiev_ua-123456789-1108422025-02-09T14:55:32Z Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste Методики та технології визначення вмісту ізотопів урану та плутонію в радіоактивних відходах Методики и технологии определения содержания изотопов урана и плутония в радиоактивных отходах Kirichenko, V.V. Makhnenko, L.A. Noga, V.I. Application of the nuclear methods In this review, the issues of radiation and nucleus safety at dealing with nuclear waste (RW) are considered. The examples of already worked out technologies on definition of the isotopes contents of uranium and plutonium in radioactive waste are adduced; the possibilities of implementation of techniques with application of electron linac are shown. Розглянуто питання забезпечення радіаційної та ядерної безпеки при роботі з радіоактивними відходами (РАВ). Наведено приклади вже розроблених технологій з визначення вмісту ізотопів урану і плутонію в радіоактивних відходах, показано можливості реалізації методик з використанням лінійних прискорювачів електронів. Рссмотрены вопросы обеспечения радиационной и ядерной безопасности при обращении с радиоактивными отходами (РАО). Приведены примеры уже разработанных технологий по определению содержания изотопов урана и плутония в радиоактивных отходах, показаны возможности реализации методик с применением линейных ускорителей электронов. 2003 Article Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste / V.V. Kirichenko, L.A. Makhnenko, V.I. Noga // Вопросы атомной науки и техники. — 2003. — № 2. — С. 111-115. — Бібліогр.: 11 назв. — англ. 1562-6016 PACS: 28.41.Kw https://nasplib.isofts.kiev.ua/handle/123456789/110842 en Вопросы атомной науки и техники application/pdf Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
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Application of the nuclear methods Application of the nuclear methods |
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Application of the nuclear methods Application of the nuclear methods Kirichenko, V.V. Makhnenko, L.A. Noga, V.I. Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste Вопросы атомной науки и техники |
| description |
In this review, the issues of radiation and nucleus safety at dealing with nuclear waste (RW) are considered. The examples of already worked out technologies on definition of the isotopes contents of uranium and plutonium in radioactive waste are adduced; the possibilities of implementation of techniques with application of electron linac are shown. |
| format |
Article |
| author |
Kirichenko, V.V. Makhnenko, L.A. Noga, V.I. |
| author_facet |
Kirichenko, V.V. Makhnenko, L.A. Noga, V.I. |
| author_sort |
Kirichenko, V.V. |
| title |
Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste |
| title_short |
Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste |
| title_full |
Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste |
| title_fullStr |
Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste |
| title_full_unstemmed |
Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste |
| title_sort |
techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste |
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
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2003 |
| topic_facet |
Application of the nuclear methods |
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https://nasplib.isofts.kiev.ua/handle/123456789/110842 |
| citation_txt |
Techniques and technologies of definition of the contents of uranium and plutonium isotopes in radioactive waste / V.V. Kirichenko, L.A. Makhnenko, V.I. Noga // Вопросы атомной науки и техники. — 2003. — № 2. — С. 111-115. — Бібліогр.: 11 назв. — англ. |
| series |
Вопросы атомной науки и техники |
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2025-11-27T01:27:18Z |
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TECHNIQUES AND TECHNOLOGIES OF DEFINITION OF THE
CONTENTS OF URANIUM AND PLUTONIUM ISOTOPES IN
RADIOACTIVE WASTE
V.V. Kirichenko, L.A. Makhnenko, V.I. Noga
National Science Center “Kharkov Institute of Physics and Technology”, Kharkov, Ukraine
In this review, the issues of radiation and nucleus safety at dealing with nuclear waste (RW) are considered. The
examples of already worked out technologies on definition of the isotopes contents of uranium and plutonium in
radioactive waste are adduced; the possibilities of implementation of techniques with application of electron linac
are shown.
PACS: 28.41.Kw
1. SOME ASPECTS ON THE HANDLING OF
RADIOACTIVE WASTE
First of all, it is about safeguarding a radiation
security. According to the Radiation Safety Standards
and main sanitary regulations, the firm radioactive
waste (RW) is considered to be radioactive in case its
activity makes more than 10−8 Ci/kg [1]. With provision
of specific activities for 238U and 235U it corresponds to
concentrations of 3·10−5 g/g and 4.7·10−6 g/g. The
liquid RW are considered to be radioactive, if the
contents of some radionuclide or mixture of several
radionuclides exceeds acceptable concentration levels
established for water. So the liquid RW on value of a
specific activity is subdivided into following categories:
– radioactive waste with low activity-is lower than
10−5 Ci/l;
– radioactive waste with mean activity-from 10−5 up
to 1 Ci/l;
Secondly, the safeguarding of nuclear safety is the
main issue in nuclear power engineering. In this
direction the researches are conducted and the different
aspects of radioactive waste handling and its
environmental impact are discussed.
So, in article [2], the conditions, which may cause a
self-sustaining chain reaction in a process of handling of
the RW possessing small quantities of fission stuffs, are
considered. The typical waste from plants producing
HGA is analyzed as well as firms of a fuel cycle such as
NPO "Radon", where the waste possessing fissile stuff
is stored for long term and prepared for storage. Liquid
waste with concentration of uranium of 1-5 Ci/l also
refers to them. The similar situation can arise also at
other plants of a fuel cycle. Even within low specific
contents of fission stuffs in huge volumes, forming
thousand cubic meters, the probability of originating of
self-sustaining chain reaction of fission is not expelled.
The self-sustaining nuclear reaction became possible at
the contents~3 g of 235U on 1 kg.
As at process and storage the contents of fissile
stuffs in waste can change (increase), the originating a
self-sustaining nuclear fission reaction is possible in
certain conditions. That is why a systematic analysis of
nuclear safety of all RW handling system is
indispensable, which is split into three phases:
− the analysis of a radioactive waste from the point
of view of danger of originating of self-sustaining chain
reaction of fission;
− the analysis of technological processes of conversion;
− the analysis of nuclear safety at long-time storage
of processed waste;
All kinds of waste are divided into two groups by
characteristic of material in order to define criterion of
nuclear safety. The waste, containing mainly graphite
belongs to the first group, the waste of the second one
mainly contains hydrogenous moderators. In work [3] it
is proposed to use surface density of fission stuffs as
criterion of nuclear safety for storehouses. In Table 1
the surface density for different compounds of uranium
and plutonium is adduced.
The analysis of nuclear safety of storehouses, in
which barrels with a volume of 200 l, diameter of
560 mm and thickness of a steel wall of 1,5 mm are
arranged closely in four circles by height, shows that in
order to avoid the self-sustaining chain reaction of
fission, each barrel should contain not more than 50 g of
plutonium and up to 80 g 235U.
These conditions are provided for firm waste with
low activity NPO "Radon". However, the volume of
waste decreases in 70…100 times during incineration
and it can move over to category of the waste with mean
activity.
Therefore, it is necessary to carry out analysis on the
contents of fission stuffs before incineration of waste
with low activity.
In case of liquid waste the safe concentration of
aqueous solutions of uranium and plutonium makes 9
and 7 g/1 accordingly. However, there is a probability
of fission stuffs sedimentation and obtaining of large
concentration that also demands the analysis of their
contents.
In work the typical waste is reviewed, which is
supposed to be stored or to be sent for processing in
NPO "Radon" and the calculations for definition of the
secure specific contents 235U with regard for content of
water (Table 2) are adduced.
Besides the rate of fission stuff concentration, the
chemical, mechanical and physical processes within
which the fission stuffs are separated from nuclides
absorbing neutrons are important in order to determine a
PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2003, № 2.
Series: Nuclear Physics Investigations (41), p. 111-115. 111
probability fro originating of self-sustained fission chain
reaction.
Table 1. Secure and critical surface density of
fission stuffs (g/см2 235U or 239Pu)
Connection Critical Secure
239Pu + H2О 0,2 0,14
U∗+ H2О 0,37 0,26
U∗∗+ H2О 0,5 0,35
239Pu + C 0,036 0,025
U∗+ C 0,052 0,036
U∗∗+ C 0,06 0,042
Note: uranium is enriched 90 and 5% on 235U
accordingly
Table 2. The secure specific contents of fission stuffs
for firm waste
Waste
Elemental
composition,
mass lobe of
components,
%
Enrich-
ment of
uranium,
%
Secure
specific
contents
of waste,
235Ug/кg
Gum
С 70-90
Н 3-10
О 1-10
S 3-10
4,4
90
0,78
0,48
Graphite С~100 4,4
90
0,09
0,08
Ceramic of
boards
О 50-70
Si 20-30
Al 10-20
Fe 1-2
4,4
90
3,6
2,1
Polyethylene
items
С 86
Н 14 4,4 12
Fluoroplastic
F 41-76
C 21-24
H 0-7
Cl 0-30
90
4,4
13,5
7
Organic
glass
С 60-80
Н4
О 10-30
90
4,4
90
6,9
4,3
3,9
Zirconium
waste
N 3
Zr 100
4,4
90
1,6
0,9
Plastic,
tissue of
PHV
С 38
Н 5
Cl 57
4,4
90
38
8,1
In October 1999 the International conference
TOPSEAL- 99, which was organized by Belgian and
European nuclear companies at support of the American
nuclear company, IAEA and Agencies on atomic
engineering of countries OECD (NEA) was held in
Antwerp (Belgium) [4]. The representatives from 22
European countries and also from Egypt, Russia, the
USA, Taiwan, Southern Korea participated in it. The
main subject of the conference was creation of
international storehouse for the spent fissile material.
Records of the conference contain short information on
status of RW dumping for the last 10 years as well as
the prospects of a research direction by treatment of the
RW. The following activities are planned:
– formation of general approaches for treatment of
the RW;
– working out of technical measures on
environmental protection, safety and stable exploitation;
– working out of the project of storehouse for the
long-lived RW, in particular, prolongation of activities
aimed to solve existing technical problems and to
coordinate technical and legal issues between the
organizations - participants.
More than 50 projects on the RW treatment
problems for the total amount of around €37 millions
were completed in the period 1994-1998. These projects
concerned mainly the following subjects:
– aspects of safety at RW dumping;
– field experiments on the underground exploratory
installations;
– research of features of the main technological
processes of RW treatment and other.
The field experiments were conducted in Belgium
on three underground trial installations in different
geological conditions and with the purpose of:
– check and demonstrating of the concepts of
dumping;
– filling and seal of storehouse;
– monitoring for long-term condition a component
of storehouse.
2. SITUATION IN UKRAINE
In Ukraine the problem of the spent fissile material
treatment appeared in 1997, when the exportation of
spent fissile to Russia for processing and dumping was
stopped [5] (in 1997, only 4,6% from the existing
amount of spent HGA accumulated on atomic power
stations (APS) and research reactors was sent to
Russia).
At Zaporozhye APS it is planned to create a
storehouse of a dry type in connection with a critical
situation on conventional storage of exhaust fissile
material in basins of exposure.
The main producers of a radioactive waste in
Ukraine and places of its concentration for today are:
− APS (spent fissile material);
− industry on a mining of uranium and process
industry (65,5 mill. t of radioactive waste is
accumulated);
− medical, scientific, industrial and other firms;
− the Ukrainian state association "Radon" (more than
5000 m3 of radioactive waste is accumulated);
− the zone of disposal Chernobyl’ APS (more than
1,1 bill. m3 of a radioactive waste).
The main objects of accumulation of the greatest
amount of the RW with high activity in Ukraine are the
nuclear stations, on which its partial primary processing
and temporary storage take place.
The radioactive waste at APS consists of liquid and
firm waste. The liquid waste are formed as a result of
disturbance of hermetic sealing of a primary loop, sinks
112
per head, labs, regeneration waters of special water
purifying, and at realization of decontamination
activities. The product of processing of a liquid
radioactive waste-“the bottom remainder» is stored as it
is or it is dabbed in order to decrease volume by a
method of evaporation. At all APS there is no full work
cycle of primary processing of liquid radioactive waste.
Only at Zaporozhye and Khmel’nitskiy APS the
evaporation up to salt content of 1500…1600 g/l is
carried out. At the rest of APS, liquid radioactive waste
is stored as “distillation residue", which does not meet
the requirements stipulated in the norms and rules of
treatment of liquid radioactive waste.
The firm radioactive waste is formed as a result of
maintenance and repair of generating sets. On January
1, 1998 in storehouses of APS in Ukraine, there were
261126 m3 of a firm radioactive waste and 25216 m3 of
“distillation residues".
3. OBJECT “SHELTER”
Now fissile material is in object "Shelter" arranged
in five modifications:
– pieces of an active zone;
– fuel as dust with the comparative sizes of
fragments from 1 micron up to hundreds of microns;
– stuffs keeping fuel, which represent glassy mass
formation in consequence of interaction of molten fuel
with structural materials;
– solvable salts of uranium and plutonium, the
concentration of uranium in which is 0,3 g/l;
– solvable compounds of uranium and plutonium,
which has sedimented.
Isotopes of cesium, strontium, plutonium, uranium
and americium represent the main radionuclides.
On weight the stuffs keeping fuel, in percentage
terms make: uranium oxides up to 1…8%, potassium –
1-2%, calcium – 4…10%, magnesium − 3…7%,
aluminum – 2…12%, ferry lactase − 3…10%,
zirconium − 2…4%, silicon-up to 60% and more. The
congestions of masses containing fuel in the "Shelter"
present nuclear danger conditioned by a probability of
origination of self-sustaining chain reaction. Under
influencing of different causes and due to physical-
chemical processes, the state and the properties of the
masses containing fuel is changing which makes
radiation safety situation at the "Shelter" worse. With
the passage of time one may observe modification of the
structure and properties of the masses containing fuel,
which is conditioned:
– by appearance of cracks and decay of lava on large
enough chunks;
– by destruction of lava with formation of
radioactive dust;
– by interaction of alkali contained in water, with
radionuclides and by formation of new solvable
compounds.
4. METHOD FOR DETECTION OF THE
CONTENTS OF TRANSURANICS IN
RADIOACTIVE WASTE
In France in CEA-DRN-DER- SSAE and DGA-
DRET-ETCA-DPN the technique for detection of the
contents of transuranics with the help of a electrons
linac is being worked out. The method founded on
results from counting photofission-induced delayed
neutrons from transuranics [6]. In activity, the linac of
electrons with energy up to 30 MeV, mean current of
the beam 140 μA, repetition frequency ranging from
6,25 up to 400 Hz and pulse width 2,5 μs was used. The
main problem at debugging of the techniques was a
neutron background, the life-time of which was about
20 ms. In this connection, the test-pieces of the RW
were placed in protection from polyethylene and
cadmium. Neutron detectors for a monitoring of
photoneutrons and neutrons of fission were also placed
here. In activity, there were 5 samples used: U-Pu with
the contents of uranium of 3,83 g and plutonium of
1,9 g accordingly; samples of 238U (weight 100, 194,
292 g;) sample of 235U (weight 1,9 g). Samples were
placed in cylindrical units from polyethylene with
diameter of 10 cm and length of 20 cm and from glass
with diameter of 10 cm both height of 9 cm and
concrete with diameter of 56 cm and height of 110 cm
with density 0.95, 1.70, 2.35 g/cm3 accordingly. In
Table 3 the minimum weights in grams are shown,
which were registered in the given experiment.
Table 3
Element Matrix
(СН2)n SiO2 Concrete
UPu 0,024 0,003 0,029
235U 0,016 0,027 0,058
238U 0,052 0,052 -
The obtained values of minimum weights for
matrixes U-Pu and 235U, determining sensitivity of
technique, correspond to concentrations 8,94·10−7 and
1,77·10−6 g/g.
5. TECHNOLOGIES
The company SGN and department of physical
researches (DRP) of the French commission on an
atomic energy (CEA) conduct intensive developments
on creation of engineering of the active and passive
analysis on definition of the contents of fissile stuffs in
firm and fluid radioactive waste. The necessity of
development of methods of the fissile analysis is
conditioned by the following facts:
– low level of surface contamination in storehouses
(some milligrams PuO2);
– greater amount of containers, contents of which is
necessary to analyze in short time;
– the development of technologies of a
nondestructive examination is based on implementation
of neutron-source 252Cf and neutron generators [7].
"COSAC" SYSTEM FOR 20-LITER BAGS
This system is designed for measurement of waste
with very low activity located in 20 l volumes with a
113
mild matrix. The main principle of the given system is
the activation by neutrons from 252Cf of a source with
the subsequent registration a gamma-quanta and
neutrons of fission. The system "Cosac" includes a
source and detectors, and also movable protection for a
source (Fig. 1). Usage of gamma - detectors allows
logging 1 mg of plutonium PWR during 600 s. Owing
to the neutrons of fission the low limit of detecting
makes 13 mg of plutonium PWR.
Fig. 1. Cosac system at CEN/Cadarache
THE BANCO SYSTEM FOR 220-LITER DRUMS
The system is shown in a Fig. 2, which works in a
mode of the passive analysis. The neutron counters and
gamma-spectrometer simultaneously scan along a
vertical axis of a rotated barrel. For mild matrixes with
density 0,2 limits of detecting make about 10 mg of
plutonium for fuel PWR and about 40 mg in a mode of
coincidence. In active version the neutron-source from
252Cf with intensity 106 n/s will be used. The neutrons of
fission are detected 3He-detectors. In this case limits of
detecting make 30mg 235U and 200 mg of plutonium for
fuel PWR. A time of an exposition 1000 s make.
Fig. 2. Banco system at CEN/Cadarache
5. NSC “KIPT”
In NSC KIPT on the basis of a linac complex of
electrons LYE-300 for problem solving on detection of
the contents of uranium isotopes and other fission stuffs
in the RW the pulse neutron-source with intensity
1012 n/s was constructed. The trial experiments were
conducted on the electron beam with energy
Ee=20 MeV, mean current Ie = 2 µA and at frequency of
50 Hz. After a rejecting magnet the beam was routed on
the leaden converter by thickness 4 cm, which served
the neutron-making target [8]. After the target the
moderator from polyethylene with the thickness of 8 cm
was established. All-band detector Mc-Kibben was used
for registration of neutrons of fission. Delaying neutrons
of fission between impulses of the accelerator with time
interval of 4 ms after a synchro-pulse were basically
registered during this trial. As the RW was used 10 kg
of sand with samples of uranium of different weight
with 2% by enrichment. At an exposure time equal to
600 s the minimum contents equal to 0.012 g 235U was
registered which corresponds to concentration 1.2·10−
6 g/g.
The purpose of the following work was carrying out
of experiments and development of techniques to
analyze concrete samples on the contents of 238U in
them, which is necessary to solve problems linked with
liquidation of Chernobyl catastrophe consequences
[9,10]. The experiment was conducted under the same
conditions, as the previous one. Concrete blocks with
the weight of 0.5 kg with 2% enriched uranium
introduced in them were used as samples. Samples from
114
metal uranium 2% enriched were also used in the
experiment as calibrating samples. From results of
comparison of yields of the neutrons from concrete and
calibration samples it was shown that under given
conditions of the experiment it is possible to safely
identify up to 10 g of 238U in concrete. Now with the
purpose of decreasing background the special stand on
direct output linac (Fig. 3) is built. The experiments
conducted on a hem with the same concrete samples,
have allowed reducing detection limit 238U up to 300 mg
and on 235U up to 1 mg which forms accordingly 6·10−4
and 2·10−6 g/g.
Fig. 3.The scheme of the accelerator equipment
1. Section of a linac.
2. Rejecting magnet (35°, removed).
3. Doublet of quadruple lenses.
4. Collimator - monochromator of a beam.
5,9. Inductive transient-time sensors of a current.
6,11. Faraday cups with removed absorbers.
7,12. Screens with fluorescing cover.
8. The trolley conveyor for moving of samples.
10. Doublet of short-focus quadruple lenses.
13. Ionization transient-time sensor of a current and
position of a beam.
14. The removed neutron-making target air-cooled
(target is established on mobile desktop).
15. Tested the sample of radioactive wastes.
16. Mc-Kibben detector.
17. Combined protection of the counter (paraffin,
cadmium).
6. CONCLUSIONS
Now on the treatment to the RW the large
development was received by industrial technologies,
founded on application of neutron-sources on the basis
252Cf and neutron generators. The electrons linacs will
be used for the present only for debugging techniques
on detection of small quantities 235U and 239Pu in
different matrixes. Nevertheless, problem on definition
of concentration is transuranic are rather varied both
from the point of view of a radiation safety, and from
the point of view of nuclear safety. The special value
these problems have for Ukraine, as huge quantity of a
firm and fluid radioactive waste of a nuclear industry
and Chernobuly APS is accumulated, which require
inventory. The pulse neutron-source with powerful
neutron flux is indispensable for this purpose, which can
be received on the electron linac. The experiments with
large volumes of a radioactive waste (200 l) on beams
of neutrons and gamma-quanta are now planned [11].
REFERENCES
1. Standard of a radiation safety NRB 76/87 and
main sanitary regulations of activity with
radioactive materials and other sources ionizing
radiations. Moscow: “Energoatomizdat”, 1988,
156 p. (in Russian)
2. О.V. Sichkaryk, L.I. Chkyaseli. Nuclear
safety at the treatment with a radioactive waste
keeping fission stuffs // Atomic Energy. 2000,
v. 88, №5, p. 362-370.
3. J. Anno, M. Simonneau, D. Gnerre.
Criticality safety of Pu contaminated carbon waste
in 100 L steel drums. In: The Fifth Intern. Conf. On
Nuclear Criticality Safety, v. II, Albuquergue, New
Mexico, USA, 1995, p. 1129-1135.
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V.V. Kirichenko, L.A. Makhnenko, V.I. Noga
Waste
Gum
2. SITUATION IN UKRAINE
3. OBJECT “SHELTER”
Table 3
6. CONCLUSIONS
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