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United States Patent (19) 11 Patent Number: 4,721,596 Marriott Et Al

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United States Patent (19) 11 Patent Number: 4,721,596 Marriott Et Al United States Patent (19) 11 Patent Number: 4,721,596 Marriott et al. (45) Date of Patent: Jan. 26, 1988 54 METHOD FOR NET DECREASE OF New Scientist, 7/77, pp. 14-16, Steinberg. HAZARDOUS RADIOACTIVE NUCLEAR CONF-760622-3, "Actinide Transmutation Studies: A WASTE MATERALS Review”, Croff, 6/76, pp. 1-14. (75) Inventors: Richard Marriott, Detroit, Mich.; BNWL-1900 (vol. 1), 5/74, Schreider et al., pp. Frank S. Henyey, San Diego; Adolf 1.42-1.45, 1.67. R. Hochstim, La Jolla, both of Calif. Huse et al., "Fusion-Fission Energy Systems: Some Utility Perspectives', ERDA-4, Dec. 3, 1974, pp. 73 Assignee: Perm, Inc., La Jolla, Calif. 27-61. (21) Appl. No.: 613,013 Tenney, “A Tokamak Hybrid Study," CONF-760733, pp. 71-80. 22 Filed: May 22, 1984 Rose et al, "Tokamak Antinide Burner Design Study', US-USSR Symposium of Fusion-Fission Reactors, Jul. Related U.S. Application Data 13-16, 1976, pp. 91-115. 63 Continuation of Ser. No. 455,046, Jan. 3, 1983, aban 'Alternatives for Managing Wastes From Reactors and doned, which is a continuation of Ser. No. 100,658, Post-Fission Operations in the LWRFuel Cycle', ER Dec. 5, 1979, abandoned. DA-76-43, vol. 4. 51) Int. Cl." .......................... G21G 1/02; G21G 1/06 "A Radioisotope-Oriented View of Nuclear Waste 52 U.S. Cl. .................................... 376/189; 376/169; Management', A. F. Rupp, ORNL-4476 (1972). 376/170; 376/184; 376/186; 376/158 "A Re-Examination of the Permanent Disposal of Ra 58) Field of Search ............... 376/184, 189, 158, 170, dioactive Waste', Marriott et al RIES 75-106 (1975). 376/146, 169, 186 "Advanced Waste Management Studies Progress Re port 8, BNWL-B-223 (1973), Editor A. M. Platt. (56) References Cited "High Level Radioactive Waste Management Alterna U.S. PATENT DOCUMENTS tives”, BNWL-1900, vol. 4 (1974). 2,837,475 6/1958 Newson . "Neutron-Induced Transmutation of High-Level Radi 3,175,955 3/1965 Cheverton. oactive Waste', ORNL-TM-3964, H. C. Claiborne 3,255,083 6/1966 Klahr . (1972). 3,276,963 10/1966 Pearce et al. Primary Examiner-Harvey E. Behrend FOREIGN PATENT DOCUMENTS Attorney, Agent, or Firm-Schwartz, Jeffery, Schwaab, 620485 5/1961 Canada ................................ 376/158 Mack, Blumenthal & Evans 224.9429 5/1974 Fed. Rep. of Germany . (57) ABSTRACT 802971 10/1958 United Kingdom. 1035078 1/1960 United Kingdom................ 376/189 A method for decreasing the amount of hazardous radi oactive reactor waste materials by separation from the OTHER PUBLICATIONS waste of materials having long-term risk potential and Nuclear Eng. Int., vol. 23, No. 266, 1/78, pp. 40-43, exposing these materials to a thermal neutron flux. The McKay. utilization of thermal neutrons enhances the natural Nuclear Technology, vol. 42, 1/79, pp. 34-50, Berwald decay rates of the hazardous materials while the separa et al. tion for recycling of the hazardous materials prevents Neclear Technology, vol. 42,2/79, pp. 180-194, Parish. further transmutation of stable and short-lived nuclides. Trans. ANS, 6/77, pp. 70, 71, Parish et al. Trans ANS, 6/77, pp. 293,294. 15 Claims, 38 Drawing Figures NEUTRONS WASTE TO MANTAN PRODUCTs NEUTRONS CHAIN REACTION FUTURE POSSILITY NEUTRONS FOR NSURONS FROMNO FISSION SOURCE TRANSMUTATIO (e.g., FUSON) HIGH FLUX TRANSMUTATION CHEMCAL/PHYSICA WASTE SEPARAON ReATMENT CYCLE "GOOD" SUBSTANCES "BAO" STORAGE SUBSTANCES DISPOSAL U.S. Patent Jan. 26, 1988 Sheet 1 of 32 4,721,596 FISSION NEUTRONS WASTE TO MANTAN ENERGY PRODUCTS NEUTRONS CHAIN REACTION FUTURE POSSIBILITY NEUTRONS FOR NEUTRONS FROM NO FISSION SOURCE TRANSMUTATION (e.g., FUSION) HIGH FLUX TRANSMUTATION CHEMICAL/PHYSICA WASTE SEPARATION TREATMENT CYCLE "GOOD" SUBSTANCES BAD STORAGE SUBSTANCES DISPOSAL fig. 1 U.S. Patent Jan. 26, 1988 Sheet 2 of 32 4,721,596 WOOLN||NOCHOSILNE U.S. Patent Jan. 26, 1988 Sheet 3 of 32 4,721,596 BETA DECAY SOTUPE NEUTRO YELDCAPTURE BETA DECAY HALF LIFE IN HOURS NEUTRON CAPTURE CROSS SECTION IN BARNS U.S. Patent Jan. 26, 1988 Sheet 4 of 32 4,721,596 O IO IO IO IO 4. IO IO IO IO IO 9 ty2 (YEARS) fig. 5 TIME TO DECAY TO ACTIVITY OF HALF THAT OF 238 AS A FUNCTION OF HALF LIFE THE DOTS ON THE CURVE REPRESENT FESSION PRODUCTS U.S. Patent Jan. 26, 1988 Sheet 5 of 32 4,721,596 OO 7 7 FISSIONS NEUTRON RADATIVE CAPTURES CAPTURES 7 NEUTRONS 27 NEUTRONS NEUTRONS ABSORBED N U238 NEUTRONS ABSORBED IN 2OO MODERATOR FISSION PRODUCT NUCLE NEUTRONS LOST FROM REACTOR 35 65 HIGH RSK STABLE OR POTENTIAL SHORT LIVED NEi For NUCLE NUCLE TRANSMUTATION fig. Ei U.S. Patent Jan. 26, 1988 Sheet 6 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 7 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 8 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 9 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 10 of 32 4,721,596 O O 6 O. Ol O 2O 3O 4O TIME (THOUSANDS OF HOURS ) fig. U.S. Patent Jan. 26, 1988 Sheet 11 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 12 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 13 of 32 4,721,596 O. O 2O 3O 4O 5O TIME (THOUSANDS OF HOURS) fig. 11 U.S. Patent Jan. 26, 1988 Sheet 14 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 15 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 16 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 17 of 32 4,721,596 1 U.S. Patent Jan. 26, 1988 Sheet 18 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 19 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 20 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 21 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 22 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 23 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 25 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 26 of 32 4,721,596 OOIO|||° BW||WOH+NOISSI-,(S}}[\OH) (NOSSld OO 3d U.S. Patent Jan. 26, 1988 Sheet 27 of 32 4,721,596 N ISOTOPE N SEPARATION Cs (STABLE) OOO 200O 3OOO 4OOO 5OOO 6OOO 7OOO TIME (HOURS) fig. 18 U.S. Patent Jan. 26, 1988 Sheet 28 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 29 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 30 of 32 4,721,596 O.4 AMOUNT OF Sm' HIOO MARGINAL NEUTRONS/REMOVAL OF Sm AVERAGE NEUTRONS/REMOVAL OF Smol O 2O 3O 4O TIME (HOURS U.S. Patent Jan. 26, 1988 Sheet 31 of 32 4,721,596 U.S. Patent Jan. 26, 1988 Sheet 32 of 32 4,721,596 - l & 3 S. rf) o S. CN O O O O O O O O O (NOSS- OO 3d) LN? OWW 4,721,596 1. 2 would permanently remove the wastes by transporta METHOD FORNET DECREASE OF HAZARDOUS tion by rocket into the sun. Two major problems face RADIOACTIVE NUCLEAR WASTE MATERIALS this technique. First the cost, and second, but more significant, there is the possibility of vehicle failure This application is a continuation of application Ser. 5 within the atmosphere leading to a highly dangerous No. 455,046, filed 1-3-83, now abandoned, which is a level of radioactive contamination. continuation of application Ser. No. 100,658, filed on A more attractive technique involves the direct trans Dec. 5, 1979, now abandoned. mutation of the dangerous waste materials by neutron BACKGROUND OF THE INVENTION bombardment into innocuous materials, or at worst 10 short lived radioactive species. Such a transmutation 1. Field of the Invention can be achieved, for example, by recycling waste prod The invention is in the field of nuclear waste control ucts back into the reactor which produced them. Such and is particularly directed toward the elimination of nuclear transformations have been discussed in the liter long-lived radioactive nuclides of nulcear reactor ature but have been found only applicable for effective Waste. 15 elimination of the actinides produced by neutron cap 2. Description of the Prior Art ture, e.g., "Advanced Waste Management Studies The difficulties encountered in attempting to safely Progress Report', 8, BNWL-B-223 (1973); H. C. Clai dispose of radioactive wastes generated by the fission borne, "Neutron Induced Transmutation of High-Level process in nuclear reactors is probably the largest single Radioactive Wastes', ORNLTM-3964, 1, 24; and cause of public resistance to the construction of nuclear 20 "High-Level Radioactive Waste Management Alterna power stations. A decade ago it was liberally estimated tives', 4, 9, BNWL 1900 (1974). The applicability of that 200,000 megawatts of nuclear generated electricity transmuting long-lived fission products as well as the would be available by 1980. Today this expectation is actinides by neutron capture in reactors has not been down by one half. A major argument against permitting regarded as practical since such a procedure reputedly the further spread of nuclear power involves concern 25 produces more long term waste than it removes. over methods proposed for disposal of the nuclear waste products. Present methods of disposal of nuclear SUMMARY OF THE INVENTION waste, which may be in the gaseous, liquid or solid state It is therefore a general object of the invention to consist either of dilution and dispersion or storage.
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