Disposal of radioactive waste by means of nuclear conversion

Nowadays radioactive waste (RW) are being buried in geologic rocks. There is an alternative method of waste disposal. It is a transmutation of radioactive isotopes into stable ones by nuclear reactions with the use of accelerators with a particle energy of 50-1000 MeV. We have shown that neutrons fr...

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Veröffentlicht in:Вопросы атомной науки и техники
Datum:2001
Hauptverfasser: Khizhnyak, N.A., Migalenya, V.Ya., Voronko, V.A.
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Sprache:Englisch
Veröffentlicht: Національний науковий центр «Харківський фізико-технічний інститут» НАН України 2001
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Zitieren:Disposal of radioactive waste by means of nuclear conversion / N.A. Khizhnyak, V.Ya. Migalenya, V.A. Voronko // Вопросы атомной науки и техники. — 2001. — № 5. — С. 188-190. — Бібліогр.: 9 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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author Khizhnyak, N.A.
Migalenya, V.Ya.
Voronko, V.A.
author_facet Khizhnyak, N.A.
Migalenya, V.Ya.
Voronko, V.A.
citation_txt Disposal of radioactive waste by means of nuclear conversion / N.A. Khizhnyak, V.Ya. Migalenya, V.A. Voronko // Вопросы атомной науки и техники. — 2001. — № 5. — С. 188-190. — Бібліогр.: 9 назв. — англ.
collection DSpace DC
container_title Вопросы атомной науки и техники
description Nowadays radioactive waste (RW) are being buried in geologic rocks. There is an alternative method of waste disposal. It is a transmutation of radioactive isotopes into stable ones by nuclear reactions with the use of accelerators with a particle energy of 50-1000 MeV. We have shown that neutrons from spallation reactions have no advantages in comparison with a hard neutron spectrum reactor technology. We have shown that during reprocessing the Th-U reactor RW, where there is a lack of actinide group, the effectiveness of proton beams and neutrons from the spallation reaction for RW disposal may be at the required level.
first_indexed 2025-12-07T17:05:41Z
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fulltext DISPOSAL OF RADIOACTIVE WASTE BY MEANS OF NUCLEAR CONVERSION N.A. Khizhnyak, V.Ya. Migalenya, V.A. Voronko National Science Center, Kharkov Institute of Physics and Technology, 1, Akademicheskaya, Str., 61108, Kharkov, Ukraine e-mail: voronko@kipt.kharkov.ua Nowadays radioactive waste (RW) are being buried in geologic rocks. There is an alternative method of waste dis- posal. It is a transmutation of radioactive isotopes into stable ones by nuclear reactions with the use of accelerators with a particle energy of 50-1000 MeV. We have shown that neutrons from spallation reactions have no advantages in comparison with a hard neutron spectrum reactor technology. We have shown that during reprocessing the Th-U reactor RW, where there is a lack of actinide group, the effectiveness of proton beams and neutrons from the spalla- tion reaction for RW disposal may be at the required level. PACS numbers: 28.41.Kw, 89.60.Ec Radioactive products are accumulated as a result of U nucleus fission in the reactors and successive radia- tion neutron captures. The problem of disposal of ra- dioactive waste from nuclear power plants has been dis- cussed in literature since the end of the 60th. On the one hand it is the most important problem the solution of which determines the development of the environmen- tally safe nuclear engineering on the Earth. A number of variants for this problem be solved has been proposed. On the other hand, each of suggested solutions is rather complex from the mechanical point of view and the suc- cessful realization causes so many problems that up till now none of proposals has been realized seriously in the world. There is only the well-known conception of ra- dioactive waste disposal by burring them in stable geo- logical rocks after hardening as glass or ceramics. The tectonic stability of these formations over at least 1000 years should permit to decrease the potential dan- ger to the acceptable level. And though the areas re- quired for their storage are relatively small (3000 m2 for 1 GW per year), the social opinion considers such a so- lution of this problem unacceptable and it is the moving force to search new more effective methods of radioac- tive waste transmutation. The solution of the problem is especially urgent in the Ukraine therefore 13 power re- actors of 12 GW produce about 30% of all the electrical energy. The single reliable and safe method of long-lived ra- dioactive nuclear waste disposal is the transmutation i.e. the conversion them into stable isotopes by neutron [1] or other radioactive radiation. Many of nuclear physical laboratories of the world are engaged now in basing this practically admissible method of transmutation but up to date none of suggested methods has been used. The dif- ficulty is due to that the quantity of radioactive nuclei in waste of the atomic industry to be transmutated is rather high and transmutation of every kind of radioactive nu- clei requires definite individual conditions, and the as- sertion of the type that it is enough to place these fission fragments into a nuclear reactor with a high neutron density to expose them to effective transmutation evi- dences on misunderstanding of this process. And the main condition is that the effective transmutation of ra- dioactive nuclei is possible only on pure isotopic tar- gets. Therefore all these variants of transmutation begin to work after waste fuels are disintegrated into separate elements and isotopes. In NSC KIPT over many years a new original method of ion mass separation is devel- oped and in our opinion this problem should be solved in the cooperation with other Institutes of the Ukraine. In [1] the problem of using fission reactors with high-energy spectrum for lowering content of isotopes such as Krypton-85, Strontium-90 and Cesium-137 was considered. In [2] the same problem was researched supposing that generators of neutrons are protons of the electronuclear installation. The application of a ther- monuclear reactor for transmutation was considered in [ 3]. All the above mentioned technologies were general- ized and studied in the well-know work [4] where fol- lowing conclusions have been made. Disposing of fission products such as Strontium-90, Cesium-137, Krypton-85, long-lived radioactive nuclei (LLRN) with transmutation as a result of multiple cy- cles of irradiation in existing now and being designed constructions of nuclear reactors is impossible due to in- sufficiently high neutron flows for the significant lower- ing of the effective half-life decay of the aggregates of these nuclides. Attainment of this aim requires to create neutron flows of about 1017 neutron/cm2sec in special reactors. Possible variants may be only electronuclear reactors, since even in thermonuclear reactors the neutron flow density will be of order lower. Moreover, the latter has not been realized and electronuclear reactors require as minimum the realization of a wide program of develop- ments. However, investigations carried out in NSC KIPT [5] show there is the inaccuracy in BNL papers quoted. For burning Cesium-137 in the intensive neu- tron flow with a density of 1017 neutron/cm2sec in the spectrum of neutrons formed on the target-convertor of the linear accelerator the radioactive capture cross-sec- tion will be strongly suppressed by parallel nuclear reac- tions and therefore the burning time of this isotope in- creases from 2 to 10 years, that is absolutely unaccept- able. Additional studies carried out has shown that Ce- sium-137 isotope can be sufficiently effectively trans- mutated in direct reactions with protons of rather low ВОПРОСЫ АТОМНОЙ НАУКИ И ТЕХНИКИ. 2001. №5. Серия: Ядерно-физические исследования (39), с. 188-190. 188 energies. That conclusion obtained by theoretical meth- ods gives the practical basis for all the problem of LLRN transmutation with proton beams of moderate en- ergies. The idea of radioactive waste transmutation has the authorship certificate [6]. It was shown earlier [6,7] that there was the princi- pal possibility for transmutation of long-lived nuclide of nuclear fuel cycle (NFC) into short-lived stable ones as a result of nuclear reactions (p, xn yp) under irradiation radiation of nuclear fuel fission products with protons of the energy lower than 50 MeV. To estimate the techno- logical possibility of transmutation (burning) using the proton accelerators of low energies (Ep<100 MeV) it is necessary to have information about nuclear constants of proceeding nuclear physical processes. In preliminary estimations the results of calculations for cross-sections of long-lived radioactive fission product burning are given and the value of the energy consumption for NFC fission product transmutation with low-energy protons is considered. To carry out the analysis of fission product transmu- tation with proton beams of the energy less than 50 MeV the calculations for functions of excitation re- actions (p, xn, yp) of on nuclei 85Kr, 88Sr, 90Sr, 99Tc, 107Pd, 133Cs, 137Cs, 151Sm have been fulfilled. Calcula- tions were made according to the statistical model of the compound nucleus taking into account the preequilibri- um decay [8]. From results obtained it follows that when 85Kr, 90Sr, 167Pd are irradiated with proton beams of the energy Ep<50 MeV, stable and short-lived nu- clides are formed. 99Tc irradiation with Ep<25 MeV proton beam results in formation of radioactive nuclei 97Тс, 96Tc and 93Mo with half-life 4.6·106 years and 3.5·103 years, respectively. During irradiation of 137Сs with Ер>30 МeV the re- action channels (р, 5n) and (p, p2n) are opened leading to production of 133Ва (Т1/2=10.54 y.) and 135Сs (T1/2=2.3·106 y.), and for 151Sm in all the energy range the production of long-lived nuclides takes place. In the process of transmutation of fissile products without isotope separation the stable isotopes of a given element will transmutate into other nuclides often being radioactive ones. Calculations results for functions of excitation of re- actions proceeding on stable isotopes 88Sr and 133Cs show that the maximum value of Т1/2 nuclides formed during proton interaction with 88Sr is 106.6 days, and in case of 133Cs it is 10.54 yeas, i.е. an additional quantity of long-lived nuclides is produced that lowers transmu- tation effectiveness. Total reaction cross-sections of 88Sr and 133Cs approach to those of radioactive nuclides of strontium and cesium that results in the additional ex- pense of an accelerated beam for reprocessing. General- ly, independently on the transmutation method the burn- ing of NFC long-lived fission products without isotope separation will lead to increasing the power consump- tion, to say nothing of possibility of new nuclide pro- duction. Under these conditions in some cases it can be more advantageously to carry out transmutation on iso- topically enriched targets. Let us consider the energy consumption for transmu- tation with low-energy protons (<50 MeV). In above- mentioned energy range the relation of probability of nuclear interactions and ionization is <10-2. Energy con- sumption for transmutation of only one nucleus will be of order of 102 Ер/ηy, where Ер is the accelerated beam energy, ηy is the efficiency of the accelerator itself. For- mation in a power reactor of one nucleus gives the use- ful energy equal to Еfηp/Y, where Еf is the decay energy, ηp is the efficiency of a reactor, Y is the output per one fission. The expedient transmutation from the viewpoint of power will be defined as follows: Efηp/Y>102 *Ep/ηy. Hence we obtain the limit on a cumulative NFC fis- sion product yield: Efηpηy/102Ep > Y. Assuming Еf=200 MeV, ηp=0.3, ηy=0.5 we obtain Y < 0.3/Ep. This equation shows that it is advantageous to use a lower energy of accelerated beam. In < 50 MeV energy range the optimal transmutation energy value is 15-20 MeV, that range where for NFC fission products the maximum of (р, 2n) reaction yield takes place and its value is near the total proton absorption cross-sec- tion. Taking Ер=20 MeV one obtains the output for which the energy balance is reached, Y=1.5%, i.е., product transmutation is energetically profitable with Y<1.5%. The result obtained is valid only for a monoisotopi- cal target. In case of transmutation without isotope sepa- ration the limitation for transmutated nuclide yield will be Y < 1.5·10-3σTcT/(Σciσi), where σT is the transmutation cross-section, ст is the transmutated nuclide concentration and ci and σi are the concentrations and total reaction cross-sections of other isotopes in the mixture. We have shown [6] that during irradiation of nuclear fuel segments with protons of the energy less than 50 MeV as a result of (р, хn yp) nuclear reactions long- lived nuclides transmutate into short-lived and stable ones with the total transmutation cross-section of 1 barn. So, for 137Cs proton beam energy of 20 MeV there are following reactions leading to stable and short- lived nuclides: 137Сs(p, n)137Ba; 137Cs(p, 2n)136Ba; 137Cs(p, 3n)135Ba; 137Cs(p, pn) 136Cs −−→ (β–, 13 суток) 136Ba; !37Cs(p, αn) 133Xe −−→ (β–, 5,29 суток) 133Cs. The calculation of these reaction cross-section made on the statistical model of the compound nucleus taking into account the preequilibrium decay gives the total cross-section of above mentioned reactions 1.03 barn. Under irradiation of radioactive nuclei with a parti- cle beam of the flow density ϕ there are two processes leading to decreasing the nucleus-target number: the process of the natural radioactive decay λ and nuclear reactions transmutating the initial nuclei into other nu- clides with the cross-section σ. In this case a half-decay period of the initial nuclide will be as Т1/2 = ln2/(λ + σϕ). At the proton 20 MeV beam density the on a cesium ВОПРОСЫ АТОМНОЙ НАУКИ И ТЕХНИКИ. 2001. №5. Серия: Ядерно-физические исследования (39), с. 188-190. 189 target 2·1017р/сm2s (about 32 mА/сm2) we obtain Т1/2=0.106 year. Since the initial amount of 137Cs (and 90Sr), contained in one ton of a spent fuel in 1000 times exceeds the activity of 1 Т natural uranium then the irra- diation time for decreasing the activity in 1000 times will be 10 Т1/2, i.е., in the given case it will be 1.06 year, that corresponds to the optimal time of transmutation as is mentioned above. The number of nuclei transmutated during the time t for the initial quantity No is N = No[1 – exp(–σϕt)]. We take No equal to the production of 137Cs in reac- tors WWER of 1000 MW (el.)–3.3·1026 nuclei per year. Then under irradiation during a day we have the amount of transmutated nuclei equal to 5.8·1024. Production of 137Cs during twenty four hours is 9·1023 nuclei. Thus, such an approach permits, in principle, to transmutate long-lived waste with processing both newly formed and storaged ones. The energy consumption is the essential moment. In the above proton energy range the relation of probability of nuclear interaction is about 10-2, i.e. to transmutate one 137Cs nucleus it is necessary to accelerate about 100 protons. Then the energy consumption for transmutation of one nucleus is Wexp.=20·100=2 GeV. So, inasmuch as for fission of one nucleus 235U in the reactor the 137Cs nucleus is formed with a probability 6·10-2, then the «useful» energy released in reactor dur- ing formation of one 137Cs nucleus we define as Wf.=200/6·10-2=3.3 GeV. Taking into account the accel- erator efficiency (<50%) and the reactor efficiency (30%) we have the relation Wexр./Wf.>4. The possibility to decrease the energy consumption for transmutation can be achieved: in the process of re- cuperating the energy of the beam passed through the target (the thickness of which must be less than the ac- celerator proton path) using an accumulation ring pro- posed by Ado et al. [9], where after passing the target the beam is accelerated again for compensation of the energy loss. It is the realization of the target as a plasma of sufficiently high density. The choice of more except- able method of decreasing the energy losses is possible only after the comparative analysis of the above meth- ods. Therefore to solve the problem of NPP long-lived waste transmutation with low- energy proton beams one should solve the following questions: •theoretical analysis of processes of proton interaction with long-lived nuclear fission products with the aim to choose an optimal beam parameters; •development of a method of decreasing unproductive losses of the beam energy in the process of transmuta- tion; •experimental investigations of transmutation processes to correct the theoretical estimations of nuclear reaction cross-sections in the process of transmutation. Finally, radioactive waste of nuclear power plants can be transmutated with the use of accelerators into stable isotopes excluding the actinide group. For this purpose two group of accelerators are necessary – accel- erators of the electric nuclear breading (proton accelera- tors with the energy of 1-1.5 GeV and average current of 0.1 А) and accelerators the construction of which is possible already nowadays (proton accelerators with the energy of 100-300 MeV and mean current 0.001 А). However, transmutation with accelerators is possible only on monoisotopic targets therefore together with ac- celerators high- efficiency separators of radioactive waste should be created. Theoretical and experimental investigations have been organized on each trend and at a physical level promising results were obtained. REFERENCES 1.M.V.Steinberg, G.Wotzak, B.Manowitz. Neutron burning of long-lived fission products for waste dispos- al. BNL-8558, Brookhaven Nat. Lab., Upton N.Y., 1958. 2.M.V.Gregory, M.V.Steinberg. A nuclear transmuta- tion system for the disposal of long-lived fission product wastes. BNL-11915, 1967. 3.W.C.Wolkenhaner. The controlled thermonuclear re- actor as a fission product burner // Trans. of the Am. Nuclear Society. 1972, p. 151. 4.H.C.Claiborn. Neutron-induced transmutation of high-level radioactive waste. 1972, ORNL-TM-3964, Oak Ridge, Tenessee. 5.V.Ya.Kostin, V.Ya.Migalenya, M.G.Shatnev, A.N.Lvov // Atomnaya energiya. 1981, v. 51, # 5, p. 336 (in Russian). 6.V.Ya.Kostin, V.Ya.Migalenya, A.N.Lvov, N.A.Khizhnyak. Authorship Certificate №950073, 704, 1982 (in Russian). 7.J.A.Ogedele. Some energetics considerations of fis- sion product transmutation with protons. Atomkernen- ergie / Kerntechnik, 1981, b. 39, p. 175. 8.M.Blann // Phys.Rev.Lett. 1972, v. 28, p. 757. 9.Yu.M.Ado et al. // Proceedings of V conference on Charged Particle Accelerator, v. 11, Moscow: Nauka, 1977, p. 317 (in Russian). ВОПРОСЫ АТОМНОЙ НАУКИ И ТЕХНИКИ. 2001. №5. Серия: Ядерно-физические исследования (39), с.188-190. 190
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institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
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publisher Національний науковий центр «Харківський фізико-технічний інститут» НАН України
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spelling Khizhnyak, N.A.
Migalenya, V.Ya.
Voronko, V.A.
2015-03-24T18:38:41Z
2015-03-24T18:38:41Z
2001
Disposal of radioactive waste by means of nuclear conversion / N.A. Khizhnyak, V.Ya. Migalenya, V.A. Voronko // Вопросы атомной науки и техники. — 2001. — № 5. — С. 188-190. — Бібліогр.: 9 назв. — англ.
1562-6016
PACS numbers: 28.41.Kw, 89.60.Ec
https://nasplib.isofts.kiev.ua/handle/123456789/79025
Nowadays radioactive waste (RW) are being buried in geologic rocks. There is an alternative method of waste disposal. It is a transmutation of radioactive isotopes into stable ones by nuclear reactions with the use of accelerators with a particle energy of 50-1000 MeV. We have shown that neutrons from spallation reactions have no advantages in comparison with a hard neutron spectrum reactor technology. We have shown that during reprocessing the Th-U reactor RW, where there is a lack of actinide group, the effectiveness of proton beams and neutrons from the spallation reaction for RW disposal may be at the required level.
en
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
Вопросы атомной науки и техники
Disposal of radioactive waste by means of nuclear conversion
Уничтожение радиоактивных отходов с помощью ядерных превращений
Article
published earlier
spellingShingle Disposal of radioactive waste by means of nuclear conversion
Khizhnyak, N.A.
Migalenya, V.Ya.
Voronko, V.A.
title Disposal of radioactive waste by means of nuclear conversion
title_alt Уничтожение радиоактивных отходов с помощью ядерных превращений
title_full Disposal of radioactive waste by means of nuclear conversion
title_fullStr Disposal of radioactive waste by means of nuclear conversion
title_full_unstemmed Disposal of radioactive waste by means of nuclear conversion
title_short Disposal of radioactive waste by means of nuclear conversion
title_sort disposal of radioactive waste by means of nuclear conversion
url https://nasplib.isofts.kiev.ua/handle/123456789/79025
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