SE429587B - PROCEDURE FOR RELEASE OF CLIFTING GASES FROM IRREDLED NUCLEAR FUEL - Google Patents
PROCEDURE FOR RELEASE OF CLIFTING GASES FROM IRREDLED NUCLEAR FUELInfo
- Publication number
- SE429587B SE429587B SE7801361A SE7801361A SE429587B SE 429587 B SE429587 B SE 429587B SE 7801361 A SE7801361 A SE 7801361A SE 7801361 A SE7801361 A SE 7801361A SE 429587 B SE429587 B SE 429587B
- Authority
- SE
- Sweden
- Prior art keywords
- nitrogen
- nuclear fuel
- fuel
- oxide
- process according
- Prior art date
Links
- 238000000034 method Methods 0.000 title claims description 27
- 239000007789 gas Substances 0.000 title claims description 12
- 239000003758 nuclear fuel Substances 0.000 title claims description 12
- 239000000446 fuel Substances 0.000 claims description 31
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims description 25
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 claims description 22
- 239000000047 product Substances 0.000 claims description 21
- 238000006243 chemical reaction Methods 0.000 claims description 20
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 claims description 15
- YZCKVEUIGOORGS-NJFSPNSNSA-N Tritium Chemical compound [3H] YZCKVEUIGOORGS-NJFSPNSNSA-N 0.000 claims description 14
- 229910052722 tritium Inorganic materials 0.000 claims description 14
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 10
- 230000004992 fission Effects 0.000 claims description 10
- 239000007800 oxidant agent Substances 0.000 claims description 10
- 239000000843 powder Substances 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 9
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 7
- 238000010494 dissociation reaction Methods 0.000 claims description 7
- 230000005593 dissociations Effects 0.000 claims description 7
- 229910052760 oxygen Inorganic materials 0.000 claims description 7
- 239000001301 oxygen Substances 0.000 claims description 7
- WZECUPJJEIXUKY-UHFFFAOYSA-N [O-2].[O-2].[O-2].[U+6] Chemical compound [O-2].[O-2].[O-2].[U+6] WZECUPJJEIXUKY-UHFFFAOYSA-N 0.000 claims description 5
- 238000007865 diluting Methods 0.000 claims description 5
- 229910052757 nitrogen Inorganic materials 0.000 claims description 5
- 229910000439 uranium oxide Inorganic materials 0.000 claims description 5
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 claims description 3
- 229910052743 krypton Inorganic materials 0.000 claims description 3
- DNNSSWSSYDEUBZ-UHFFFAOYSA-N krypton atom Chemical compound [Kr] DNNSSWSSYDEUBZ-UHFFFAOYSA-N 0.000 claims description 3
- 230000001590 oxidative effect Effects 0.000 claims description 3
- 229910052724 xenon Inorganic materials 0.000 claims description 3
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 claims description 3
- 239000013078 crystal Substances 0.000 claims description 2
- SHZGCJCMOBCMKK-KGJVWPDLSA-N beta-L-fucose Chemical compound C[C@@H]1O[C@H](O)[C@@H](O)[C@H](O)[C@@H]1O SHZGCJCMOBCMKK-KGJVWPDLSA-N 0.000 claims 2
- 241000271566 Aves Species 0.000 claims 1
- 239000000729 antidote Substances 0.000 claims 1
- 239000003795 chemical substances by application Substances 0.000 claims 1
- 238000007254 oxidation reaction Methods 0.000 description 13
- FCTBKIHDJGHPPO-UHFFFAOYSA-N uranium dioxide Inorganic materials O=[U]=O FCTBKIHDJGHPPO-UHFFFAOYSA-N 0.000 description 12
- 230000003647 oxidation Effects 0.000 description 10
- 238000012958 reprocessing Methods 0.000 description 5
- 238000002474 experimental method Methods 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- 239000008188 pellet Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000003776 cleavage reaction Methods 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- FLDALJIYKQCYHH-UHFFFAOYSA-N plutonium(IV) oxide Inorganic materials [O-2].[O-2].[Pu+4] FLDALJIYKQCYHH-UHFFFAOYSA-N 0.000 description 3
- 230000007017 scission Effects 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000005372 isotope separation Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 229910017604 nitric acid Inorganic materials 0.000 description 2
- OOAWCECZEHPMBX-UHFFFAOYSA-N oxygen(2-);uranium(4+) Chemical compound [O-2].[O-2].[U+4] OOAWCECZEHPMBX-UHFFFAOYSA-N 0.000 description 2
- 239000011343 solid material Substances 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 1
- 239000005751 Copper oxide Substances 0.000 description 1
- 101100298295 Drosophila melanogaster flfl gene Proteins 0.000 description 1
- XLYOFNOQVPJJNP-PWCQTSIFSA-N Tritiated water Chemical compound [3H]O[3H] XLYOFNOQVPJJNP-PWCQTSIFSA-N 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 101150059062 apln gene Proteins 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 238000000429 assembly Methods 0.000 description 1
- 230000000712 assembly Effects 0.000 description 1
- 238000000889 atomisation Methods 0.000 description 1
- 229910000431 copper oxide Inorganic materials 0.000 description 1
- 239000003085 diluting agent Substances 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 230000009931 harmful effect Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000003380 propellant Substances 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000005496 tempering Methods 0.000 description 1
- 230000004584 weight gain Effects 0.000 description 1
- 235000019786 weight gain Nutrition 0.000 description 1
Classifications
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- E—FIXED CONSTRUCTIONS
- E21—EARTH OR ROCK DRILLING; MINING
- E21B—EARTH OR ROCK DRILLING; OBTAINING OIL, GAS, WATER, SOLUBLE OR MELTABLE MATERIALS OR A SLURRY OF MINERALS FROM WELLS
- E21B7/00—Special methods or apparatus for drilling
- E21B7/26—Drilling without earth removal, e.g. with self-propelled burrowing devices
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C19/00—Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
- G21C19/42—Reprocessing of irradiated fuel
- G21C19/44—Reprocessing of irradiated fuel of irradiated solid fuel
- G21C19/48—Non-aqueous processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B25—HAND TOOLS; PORTABLE POWER-DRIVEN TOOLS; MANIPULATORS
- B25D—PERCUSSIVE TOOLS
- B25D9/00—Portable percussive tools with fluid-pressure drive, i.e. driven directly by fluids, e.g. having several percussive tool bits operated simultaneously
- B25D9/14—Control devices for the reciprocating piston
- B25D9/26—Control devices for adjusting the stroke of the piston or the force or frequency of impact thereof
-
- E—FIXED CONSTRUCTIONS
- E21—EARTH OR ROCK DRILLING; MINING
- E21B—EARTH OR ROCK DRILLING; OBTAINING OIL, GAS, WATER, SOLUBLE OR MELTABLE MATERIALS OR A SLURRY OF MINERALS FROM WELLS
- E21B4/00—Drives for drilling, used in the borehole
- E21B4/06—Down-hole impacting means, e.g. hammers
- E21B4/14—Fluid operated hammers
- E21B4/145—Fluid operated hammers of the self propelled-type, e.g. with a reverse mode to retract the device from the hole
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/28—Treating solids
- G21F9/30—Processing
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W30/00—Technologies for solid waste management
- Y02W30/50—Reuse, recycling or recovery technologies
Landscapes
- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- Mining & Mineral Resources (AREA)
- Geology (AREA)
- Life Sciences & Earth Sciences (AREA)
- Fluid Mechanics (AREA)
- Mechanical Engineering (AREA)
- Environmental & Geological Engineering (AREA)
- High Energy & Nuclear Physics (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geochemistry & Mineralogy (AREA)
- General Engineering & Computer Science (AREA)
- Plasma & Fusion (AREA)
- Automation & Control Theory (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Monitoring And Testing Of Nuclear Reactors (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
Description
mg 30136 ..,..\ -2 blir i form av tritierat vatten intimt blandat med den i anläggningen använda processvattenmängden, som är av kubikmeterstorlek. Isotop- separation av tritium från denna stora volym av vatten skulle krävas innan vattnet skulle kunna utsläppas såsom vätska eller ånga. Efter- som isotopseparering av tritium i sådana vattenvolymer icke är prak- tiskt genomförbar är det nödvändigt att utveckla en metod för avläg- snande av flyktiga klyvningsprodukter från bestrålat bränsle före upparbetningen i vattenlösning. l Problemet att avlägsna flyktiga klyvningsprodukter från be- strålat bränsle uppkommer vid upparbetning av bestrålat urandioxid- bränsle och/eller bestrâlat blandoxider, dvs U02 och PuO2; Problemet att avlägsna det flyktiga klyvningsprodukterna ökas av det förhållan- det att de flyktiga klyvningsprodukterna inneslutas i kristallgitt- ret i det bestnålade bränslet och sålunda icke kan avlägsnas genom malning eller pulvrisering av bränslet. I Ett förfarande för avlägsnande av flyktiga klyvningsprodukter från bestrâlat bränsle har utvecklats av Oak Ridge National Laborato- ries, USA, och benämnes “voloxidation" och beskrives i Oak Ridge National Laboratories Report ORNL-Th-3723. Voloxidering är en process för oxidering av bestrålat bränsle i närvaro av syre vid en reglerad temperatur för bildning av ett mycket fint pulver av U3O8. Voloxi- deringsprocessen är känslig för temperaturen, och man har uppskattat att i en stor och konversiell anläggning måste reaktionstemperaturen hållas inom ett snävt intervall, förmodligen vid ca 480°Cg plus eller minus l0°C. På grund av det kritiskt snäva temperaturområdet skulle svårigheterna att driva upparbetningsanläggningar i stor skala ökas.-Föreliggande uppfinning avser ett förfarande för fri- göring av de flyktiga klyvningsprodukterna från bestrâlat bränsle inom en kommersiellt acceptabel tidrymd och under kommersiellt accep- tabla processbetingelser varigenom man uppnår en väsentlig minskning av kostnaderna vid upparbetningen av bestrålade kärnbränslen. mg 30136 .., .. \ -2 in the form of tritiated water is intimately mixed with that in the plant use the process water quantity, which is of cubic meter size. Isotope- separation of tritium from this large volume of water would be required before the water could be discharged as liquid or vapor. After- isotope separation of tritium in such volumes of water is not practical practically feasible, it is necessary to develop a method of volatile fission products from irradiated fuel before reprocessing in aqueous solution. The problem of removing volatile cleavage products from Radiated fuel is produced during the reprocessing of irradiated uranium dioxide fuel and / or irradiated mixed oxides, ie UO2 and PuO2; The problem the removal of the volatile cleavage products is increased by the that the volatile cleavage products are enclosed in crystal lattice in the distilled fuel and thus can not be removed by grinding or pulverizing the fuel. IN A process for removing volatile fission products from irradiated fuel has been developed by the Oak Ridge National Laboratory ries, USA, and is termed "voloxidation" and is described in Oak Ridge National Laboratories Report ORNL-Th-3723. Voloxidation is a process for oxidation of irradiated fuel in the presence of oxygen at a regulated temperature to form a very fine powder of U3O8. Voloxy The tempering process is sensitive to temperature, and has been appreciated that in a large and conversion plant the reaction temperature must kept within a narrow range, probably at about 480 ° Cg plus or minus 10 ° C. Due to the critically narrow temperature range the difficulties of operating reprocessing plants would be large The present invention relates to a method for freeing making the volatile fission products from irradiated fuel within a commercially acceptable period of time and during tabla process conditions whereby a significant reduction is achieved of the costs of reprocessing irradiated nuclear fuels.
Föreliggande uppfinning avser allmänt en process för oxidering av bestrålade kärnbränslen för frigöring av de flyktiga klyvnings- produkterna, dvs jod, xenon, krypton och tritium. Bestrâlad uran- dioxid eller blandoxidbränslen okideras med en kväveoxid, exempelvis kvävedioxid. Kvävedioxid står vid reaktionstemperaturen vid denna I process vid en med sina dissooiationsprodukter, kvävemonoxid och syre.The present invention relates generally to an oxidation process of irradiated nuclear fuels for the release of the volatile fission products, ie iodine, xenon, krypton and tritium. Irradiated uranium dioxide or mixed oxide fuels are oxidized with a nitric oxide, for example nitrogen dioxide. Nitrogen dioxide is at the reaction temperature at this I process at one with its dissociation products, nitrogen monoxide and oxygen.
Oxidationsmedlet kan sålunda tillsättas såsom kvävedioxid, såsom dis- sociationsprodukten av kvävedioxid (kvävemonoxid och syre) eller så- som en blandning av kvävedioxid och dess dissociationsprodukter. Oxi- 7801361-2 dationsmedlet kan utspädas med en gas exempelvis kväve eller kväve- monoxid utan någon väsentlig skadlig effekt. Oxidationsreaktions- temperaturen kan vara från ca 325°C till 800°C och företrädesvis mellan 350°C och 780°C. Reaktionen jämföres företrädesvis vid en temperatur inom omrâdet 3500 - 650°C.The oxidizing agent can thus be added as nitrogen dioxide, such as the social product of nitrogen dioxide (nitrogen monoxide and oxygen) or as a mixture of nitrogen dioxide and its dissociation products. Oxi- 7801361-2 the diluent can be diluted with a gas such as nitrogen or nitrogen. monoxide without any significant harmful effect. Oxidation reaction the temperature may be from about 325 ° C to 800 ° C and preferably between 350 ° C and 780 ° C. The reaction is preferably compared to a temperature in the range 3500 - 650 ° C.
Oxidationsreaktionen upprätthâlles under en tidrymd som är tillräcklig för omvandling av de bestrålade bränslekutsarna till ett fint pulver med en medelpartikelstorlek av mindre än 0,105 mm och företrädesvis mindre än 0,045 M . Upphettning till reaktions- temperaturer över 800°C medför en agglomerering av det fina pulv- ret och bör sålunda undvikas.The oxidation reaction is maintained for a period of time which is sufficient for the conversion of the irradiated fuel pellets to a fine powder with an average particle size of less than 0.105 mm and preferably less than 0.045 M. Heating to reaction temperatures above 800 ° C result in an agglomeration of the fine powder. and should thus be avoided.
De bestrålade bränslepatronerna tillåtas efter avlägsnande från reaktorn i allmänhet att svalna och därefter uppskäras eller upphuggas bränslestavarna för beredning av det bestrålade bränslet för upparbetning. Det bestrålade kärnbränslet införes därefter i ett reaktionskärl och kvävedioxid enbart över i blandning med dess dissociationsprodukter bringas att passera genom reaktorn. Systemet upphettas till en reaktionstemperatur mellan 3250 och 8000 C.The irradiated fuel assemblies are allowed after removal from the reactor generally to cool and then cut or the fuel rods are chopped to prepare the irradiated fuel for reprocessing. The irradiated nuclear fuel is then introduced into a reaction vessel and nitrogen dioxide alone mixed with it dissociation products are passed through the reactor. The system heated to a reaction temperature between 3250 and 8000 C.
Under oxidationsreaktionen frigöras drivningsgaser i synnerhet tritium, i det närmaste kvantitativa mängder till avgassystemet.During the oxidation reaction, propellant gases in particular are released tritium, almost quantitative amounts to the exhaust system.
Under reaktionen oxideras U02 till bi1dHin9_aVU0¿ och/eller U308- Enligt uppfinningen kan ett bestrålat kärnbränsle, dvs U02 eller en blandning av UO2 och PuO2, införas i reaktionskärlet och oxideras med kväveoxid, exempelvis kvävedioxid eller en bland- ning kvävedioxid och dess dissociationsprodukter, syre och kväve- monoxid. Oxidationen genomföres genom att det bestrålade bränslet införes i reaktionskärlet och upphettas till en reaktionstemperatur av ca 350°'730°C i närvaro av kväveoxiden. Det bestrålade bränslet upphettas under en tidrymd som är tillräcklig för finfördelning av det bestrâlade bränslet till ett fint pulver (U308 och UO3)- RGäk“ tionstiden varierar beroende på materialvolymen i reaktorn, det upp- huggna bränslets storlek, UO2-partikelstorleken, temperaturen ocn gassammansättningen. Det fina pulvret har en medelpartikeldiameter om mindre än 0,105 mm och företrädesvis en medelpartikeldiameter av mindre än 0,045 mm.During the reaction, UO2 is oxidized to bi1dHin9_aVU0¿ and / or U308- According to the invention, an irradiated nuclear fuel, i.e. UO2, or a mixture of UO2 and PuO2, is introduced into the reaction vessel and oxidized with nitric oxide, for example nitrogen dioxide or a mixed nitrogen dioxide and its dissociation products, oxygen and nitrogen monoxide. The oxidation is carried out by the irradiated fuel is introduced into the reaction vessel and heated to a reaction temperature of about 350 ° '730 ° C in the presence of the nitric oxide. The irradiated fuel heated for a period of time sufficient for atomization of the irradiated fuel to a fine powder (U308 and UO3) - RGäk “ The reaction time varies depending on the volume of material in the reactor, the chopped fuel size, UO2 particle size, temperature, etc. the gas composition. The fine powder has a mean particle diameter of less than 0.105 mm and preferably an average particle diameter of less than 0.045 mm.
Frigjort tritium kan uppsamlas såsom tritiumgas eller kan oxideras till bildning av THO, kylas och uppsamlas såsom vätska (TN03, HTO etc).Released tritium can be collected as tritium gas or can oxidized to form THO, cooled and collected as a liquid (TN03, HTO etc).
För att visa effektiviteten av förfarandet enligt uppfinningen _ 7801361-2 oxiderades bränslekutsar i normal laboratorieutrustning. Bränsle- kutsar infördes i ett provskepp och infördes i ett förbrännings- rör. Ett termoelement användes för temperaturregleringQ En rör- ugn anordnades runt förbränningsröret för tillföring av värme till systemet. Oxidationsmedlet fördes genom förbränningsröret såsom gas. Tritium som frigjordes genom oxidationen omvandlades till THO i en kopparoxidugn och kondenserades i ett kallt finger.To demonstrate the effectiveness of the method of the invention _ 7801361-2 oxidized fuel pellets in normal laboratory equipment. Fuel- pellets were introduced into a test vessel and introduced into an incinerator pipe. A thermocouple is used for temperature control. oven was arranged around the combustion pipe for supplying heat to the system. The oxidant was passed through the combustion tube such as gas. Tritium released by the oxidation was converted to THO in a copper oxide furnace and condensed in a cold finger.
EIGí-*IPEL l 7 Prover med vikten l g av bestrålat uranoxid (UO¿) bränsle och ett blandoxidbränsle GBDZ/PuO2) oxiderades under fyra timmars tid med N02 vid 400°C.'Vid slutet av fyratimmarsperioden förelåg det bestrålade bränslet i form av ett mycket fint pulver. Det er- hållna pulvret upplöstes i 15 ml 8 molar HNO3 under mellan tre och fyra timmars tid vid l0O°C, filtrerades och därefter togs prover för bestämning av kvarvarande tritium i lösning. Ett ytterligare prov med vikten 1 g av vart och ett av de bestrålade bränslenaysom icke underkastats N02-oxidation, upplöstes direkt i 8 molar HN03 under ca fyra timmars tid vid l00°C, filtrerades och därefter togs prover för tritium såsom standardprov. De kvarvarnade filtrerade fasta materialen från både standardproven och försöksproverna upp- löstes ytterligare med 8 molar HNO3 plus 0,005 molar fluorvätesyra, och från den erhållna lösningen togs prov för bestämning av tritium- halten i de fasta materialen. Resultaten av oxidationen av de tvâ bränsleproverna anges i tabell l i det följande. 7801361-2 w m «.Q «w.Q ~oøm\~o= wmuwwflxoxwoz | HH_ø «.o~ ~oøm\~oa øumwcmuw «~.° ~H.Q ß~.o Noa umuøwflxonfloz | m°.Q °.mmH Non uumwqmuw fiumflcmum .mcflcmwfiwmcflmmmammd flmE uumwšmfi Eflfluwuu w uumm NOS m\.won~šs..fiufluv uømcdm wflwøwnm H HHQQMH ...nu w..- wnu.. 7,... 7801361-2 Av dessa resultat framgår att oxidation med NO2_av bränslet före upplösningen effektivt avlägsnade tritium från bränslet.EIGí- * IPEL l 7 Samples weighing 1 g of irradiated uranium oxide (UO¿) fuel and a mixed oxide fuel (GBDZ / PuO2) was oxidized for four hours time with NO 2 at 400 ° C. 'At the end of the four hour period there was the irradiated fuel in the form of a very fine powder. It is- The powder was dissolved in 15 ml of 8 molar HNO3 for between three and four hours at 10 ° C, filtered and then samples taken for the determination of residual tritium in solution. One more samples weighing 1 g of each of the irradiated fuel naysom not subjected to NO 2 oxidation, dissolved directly in 8 molar HNO 3 for about four hours at 100 ° C, filtered and then taken samples for tritium as standard samples. The remaining ones were filtered the solid materials from both the standard samples and the experimental samples was further dissolved with 8 molar HNO3 plus 0.005 molar hydrofluoric acid, and from the resulting solution samples were taken to determine tritium the content of the solids. The results of the oxidation of the two the fuel samples are given in Table 1 below. 7801361-2 w m «.Q« w.Q ~ oøm \ ~ o = wmuww fl xoxwoz | HH_ø «.o ~ ~ oøm \ ~ oa øumwcmuw «~. ° ~ H.Q ß ~ .o Noa umuøw fl xon fl oz | m ° .Q ° .mmH Non uumwqmuw fi um fl cmum .mc fl cmw fi wmc fl mmmammd fl mE uumwšm fi E flfl uwuu w uumm NOS m \ .won ~ šs .. fi u fl uv uømcdm w fl wøwnm H HHQQMH ... nu w ..- wnu .. 7, ... 7801361-2 These results show that oxidation with NO2_of the fuel before dissolution, tritium was effectively removed from the fuel.
Upplösningslösningen för blandoxiden samt det fasta materialen innehöll 5 % av den ursprungliga tritiumhalten.The dissolution solution for the mixed oxide and the solid materials contained 5% of the original tritium content.
EXEI-'ÅPEL 2 En serie försök genomfördes under isotermiska betingelser vid temperaturer från 300°-80000 med användning av prover av U02-bränsle- kutsar för bestämning av reaktionshastigheten. När oxidationen av- slutats var kärnbränslet omvandlat till ett finfördelat pulver och bränsleprovet visade en viktökning av 4 viktprocent. De resultat som anges på fig l erhölls.EXEI-'APEL 2 A series of experiments were performed under isothermal conditions at temperatures from 300 ° -80000 using samples of U02 fuel pellets for determining the reaction rate. When the oxidation ended, the nuclear fuel was converted into a finely divided powder and the fuel sample showed a weight gain of 4% by weight. The results indicated in Fig. 1 was obtained.
Vid försök som genomfördes vid temperaturerna 325°-600°C ut- gjorde slutprodukten ett pulver. Försök utförda vid 3509, 500° och 600°C synes vara i huvudsak ekvivalenta..In experiments performed at temperatures of 325 ° -600 ° C made the final product a powder. Tests performed at 3509, 500 ° and 600 ° C appear to be substantially equivalent.
EXEMÉPEL 3 En serie försök med konstant upphettningshastighet genomfördes för provning av effekten av utspädning av oxidationsmedlet N02, med kväve, varvid de påfig 2 visade resultaten erhölls.EXAMPLE 3 A series of experiments with a constant heating rate were performed for testing the effect of diluting the oxidizing agent NO2, with nitrogen, whereby the results shown in Fig. 2 were obtained.
Bränsleproverna utgjordes av U02-bränslestycken. Det kan observeras att reaktionshastigheten för oxidation av UO2 i N02 är förhållandevis okänslig för H2-utspädning.The fuel samples consisted of U02 fuel pieces. It can it is observed that the reaction rate for oxidation of UO2 in NO2 is relatively insensitive to H2 dilution.
EXEI-IPEL 4 _ För bestämning av inverkan av N02'“tSPäÛnifl9 På U02 0Xiå&fii0n genomfördes experiment med konstant upphettningshastighet med N02 och NO tillsatt såsom oxidationsmedelblandning med de på fig 3 visade resultaten. Det använda oxidationsmedlet utgjordes av en blandning av N02 och NO i mängdförhållandet l:l. Det kan observeras att ökande mängder av NO har en tendens att sänka reaktionshastig- heten vid oxidation av UO2 i N02.EXEI-IPEL 4 _ To determine the effect of N02 '“tSPäÛni fl9 On U02 0Xiå & fi i0n experiments were carried out at a constant heating rate with NO 2 and NO added as oxidant mixture with those of Fig. 3 showed the results. The oxidizing agent used consisted of a mixture of NO 2 and NO in the ratio 1: 1. It can be observed that increasing amounts of NO tend to slow down the reaction rate. oxidation of UO2 in NO2.
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JP (1) | JPS6034718B2 (en) |
BE (1) | BE863675A (en) |
DE (1) | DE2801744C2 (en) |
ES (1) | ES466675A1 (en) |
FR (1) | FR2379884A1 (en) |
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US3140151A (en) * | 1959-11-12 | 1964-07-07 | James R Foltz | Method of reprocessing uo2 reactor fuel |
BE611199A (en) * | 1961-12-06 | 1962-06-06 | Ct D Etude De L En Nucleaire | Process for the reprocessing of nuclear fuels, which include carbon in their structure and / or in their cladding. |
IT1034322B (en) * | 1975-03-17 | 1979-09-10 | Agip Nucleare Spa | PYROCHEMICAL SEPARATION OF PLUTUS NIUM FROM IRRAYED NUCLEAR FUELS BY THERMODECOMPOSITION IN MELTED NITRATES |
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- 1978-01-18 GB GB2020/78A patent/GB1593323A/en not_active Expired
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GB1593323A (en) | 1981-07-15 |
IT7819802A0 (en) | 1978-01-30 |
FR2379884B1 (en) | 1984-10-19 |
FR2379884A1 (en) | 1978-09-01 |
SE7801361L (en) | 1978-08-08 |
DE2801744A1 (en) | 1978-08-10 |
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DE2801744C2 (en) | 1986-12-11 |
JPS6034718B2 (en) | 1985-08-10 |
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