Concepts for the Nuclear Transmutation of Radioactive Waste From
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CCW',lISSIONF:DFLLF COXWI'I'A' Z:URO?E:E Stabilimento di IsDra CONCCP1'SFOR THE XJCLGATC?R.Ai'S'r'UTATIOI\I OF XADIOACTIVE Tr'ASY'EPR33 FISSION RFACT3RS AT ?RESF‘N'I IJNDPY DISCUSSICXC ~~,~~ ii*G~ md E.SCHXIDT presented to the JEXDR?C: aeeting Of RiS$ (!?a17 1975) bJ X.RIF:F In this reDort, a survev on the xroble-ns involved in the radioactive waste disDosa1 is given and results for ultinate disqosal techniques, as fission reactors, sgallation reactors, ;?lld fusion reactors are reviewed. - . t 5.1" Desip of Spallation Reactor 5.2. Additional Costs of Nuclear 3nergv due to Incineration lx, a Snallation Eeactor 5.3. Demands Eclr Nuclear ?easurewnts 95240002 - 2 - 1. INTRODUCTION After the fuel-oil crisis of 1973‘!74, the importance of nuclear energv for covering the energv demand increased considerablv. The Commission of the Furooean Communities established in its Wew Enerqv Policy Strategy" a nuclear target programme for the grovrth of the nuclear energv generating capacity up to the vear 2330 (Ref.1). This forecast would correspond to ,a cumulative nuclear energv generation of about This fiqare means that until the vear 2?OD about 3500 tons of fission x?oducts and 1% to~?s of actinides other than fuel have to be separated in re?rocessing Plants from spent fuel and will go to the waste. The management of this high-level radioactive waste associated with energy generation bv nuclear fission will Dresent a .formidable task to vresent and future generations of mankind. Its safe. disqosal is possibly the most important and controlling problem in the large- scale introduction of nuclear energy. ?resentlv, there does not exist a definitive solution for this qart of the nuclear fuel cvcle. ;:lhile uranium explo--~ ra~tion, develooment of enrichment slants, fuel element fabrication and design of advanced nuclea~r polger reactors were considered to be im?orta~nt activities alreadv since a~bout three decades, resroccssing and waste disposal arose as important tasks onlv during the last vears, iVOw, strong efforts are underwav in all countries with nuclear industrl! for ela~borating an acceptable radioactive xrastc disposal policv. -3- The main requirements to such a policy is that a permnent removal of the radioactive substances from manls biosDhere is guaranteed. in the bast, industrial wastes were often treated applving the orincigle that "dilution is the solution of pollution*'. Apart from the fact that presentlv mblic opinion rejects this kind of treatment even for"conventional waste", it would b.J no .mans be apolicable to radioactive :rraste, Therefore, technicians have to offer convincing concmts for the treatnent of the radioactive waste, if the ob,jcctions of public opinion against the use of nuclear enerqv shall be overcome. Concerning the disposal of the radioactive waste, three: qualitativelv different concepts .qav be distin-. guished : - storaqe - long terxl disposal. - ultimate disposal Possiblv, each of these concepts will be apglied in a~ future waste disposal ~olic;~ for different classes of wa.ste, classifying the radioactive waste e.g. in - short-lived fission products (decav to innocuous 1eveX within 39 years) - internediate-lived fission products (decav to innocuous levels within about ;03 vears) - long-lived fission products - actinides and their daughters Starace is the onlv disposal technique mulied todav for high-level radioactive waste (HAv) on an industrial scale, Xomally, it is considered as an interi>n solution and i.qp1ie.s that the waste re%ains retrievable and is under continuous surveillance. 7'hs HA:?, arising as licuid .from reprocessing slants, is stored i?: st.ainless steel tanks embedded in concrete to ~7mlts in order qain time for .mk-Ln$ d.e.finiti.ve dcci- sioiis on honi to dispose of the ~wste~ lens-t.er;r: dis;,osal refers to a disposal. of VJ?StC in salt ,ninc s , its deep buri,ai b;i injection into ground or ,undw thr: ./Ql~t?rctic:- <cc sheet, res72ective?v. Co~only ;a :>x c:I ::::‘ ;?z so-tidi fica7:i.m of the XT is s;:~bosed~. .In .rontr.Tst to thp st:7rr7 'e, the ~~~~:ste i.5 in this casf no longer considered to be recoverable. This conceat !;uaran- tec;s i: high dqree of safetv, blxt it can not be comlitel\r ercluded that the waste !rl?~~~return in an ?mcontroll?ble ~$anncr to rrim's biosohcre, if ertraordinar- events will ot-.cur D This aossibiiit- becomes the Tore ?robable, the longer the deca.~ ?crio:?s of radioactive nucl~ides to innocuous radis~tion lr?vcls are; climatic 2nd. ~e~lon~.c;1~. zlterationsT :mdificati.on of the: wy of lift o.f wn and other un~forese able: we:its coul? occur, rSnl:i the “uitimte diswsa!." of vast?: would wsult in the certaintv that no radioactive Iatcrial can return to .the biosThcrc after the tlis~osal of fastens has been success- .Flill~: accofl?lished. Tiacic?11',1( ix0 possibilities are l iim;iai.e lable as ultimate disoosal for selected. :~adio:~uc.ii.des D After nmtitiohih::! of the wast?, long-lived isotosses could be transmuted to stable or short-lived or‘ lesser ha,eard.ous ohi:.s bv Izxclcar nroresses as r,g, fission, (*:~:;,:I, (t- : .)? (r,Lj, p,?). As second solution these ecl.c,r-rted. radionuclides could be shot into the deco space (extr.z- terrestria~l dicoose!?), ':'he scope of the following consi- derations is to d:iscuss the concept of the nuclear tr~wsm- tation of radioactive wste. ~?resentlv .fission reactors, intense accelera tom and fusion rextom are inn&~ rli.scussion. -5- 2, GENERAL 3N NUCLEAR TRANSXU'TATIONS The necessitv snd feasibilitv of transmntating radioactive wastes is still under investigation, It seem, however, clear that this concept u:ill be applied only for a fevr chosen nuclides, which represent either a great radio- toxic risk or a pronounced long-tern hazard. 3ther nuclides Cl1 be disposed of by burial, The transmutation rate T of any isotope N ~sv be described by the following equation 'The first term on the right hand side regresents the natural decal1 amd the second one the elimination bv the nuclear process in consideration. In the case of neutron reactions z' qeans the effective absorotion cross section and ~5 the effective neutron flux. Sin-es' is a consta.nt for a. given neutron spectrum the onlv va.riable urhirh influences the transautation rate is the neutron flux. A feasibility study for nuclear transmutations involves consequently investigations on the Droduction of high neutron fields ahd sDectra in which ~7 rea~che s an 0ptitiu-n value, In addition, after a literature search, it becones apparent that the neutron cross section for long-lived fission Products and higher -actinides other than fuel are not well established, Finallv( technical problms mast be solved 2s e.g.mste partitioning, optinized isotope separations for nuclides to be "burned!' md daughter ,product coq?lications leading to optiqurn recvcling oeriods for given isotopes* OUIi~/C/I S,:/f;l 7 :7 5e -5- 30 TRANSXJTATION OF FISSICN PRODUCTSW FISSION REACTORS The possibility of "burning" fission products bv recvcling the!? has been s,tudied by STEINBERG and co-workers in (R~ef.2) and (Ref.'). The contribution of individual fission product nuclides to the total fission oroduct hazard of a characteristic uranium fueled LKR is shoum in Fig.1. There the hazard measure is defined as cubic meter of water needed for diluting the isotope to concentrations that the water can be used as drinking water. "iaximum.I oermissible concentra- tions are taken from the Code of Federal Regulation (USA), The fission Troducts (FP) shall be grouped into 3 classes a) volatile FF as, e.g, KR-85 b) FT which are controlling up to decav periods of about 830 years as ,e.g, Sh-90 and G-137 c) ion;-lived F? as, e.g. I-129 and TC-99. Evaluations of STEINBERG dealing with the three isotopes KR-85, SR-90 Andy CS-137 lead to the following results: It was estimated that releasing inventories of the noble gas isotope xR-85? generated bv the nuclear energy industrv, to the atmosphere will increase the back- ground count in the vear 2C3iC bv 4.2%. It appears therefore desirable to develoo a snecial treatment of this fission product. KR-85 is present in :<Crvpton wastes with a concentration of about 7:: and its a~bsorption cross-section is small (15 barns) compared with that of KR-83 (215b). In Pig;2, the burning cost for X12-85 as function of the enrichment is reproduced, It can be seen that o?timum conditions are reached if KR-85 becomes enriched to 90X. The burning costs for the optimum enriched Case are given as 0.321 mills,&:i':~he. -7- In order to avoid additional neutron burning costs or enrichment costs for SR-90 which could result from the short lived SR-39, a cooling period of about 1 vear before partitioning of SR from the gross wastes should be scheduled, Then, strontium fission products can be fed dirwtlv to the reactor. After a suitable burning period, the wastes arf processed in a chemical separa- tion plant in order to remove the barium and yttrium daughter produc.ts This qurified portion is thereafter combined with SR feed ;und recvcled through the reactor, The burning costs (onlv neutron costs) amount to 0 ” 2~;. mi 11s ~/Whe ~ Unless natural Cesium wastes are enriched in CS-137 burning does not seem feasible because of the high fission product yield (5.%), the low cross section (: = S,llb) of CS-137 and the large cross section of stable CS-133 (31b).