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Fixation of Simulated Highly Radioactive Wastes in Glassy Solids; Fixation de Dechets Simules de Haute Activite dans des Soudes Vitreux; 0424 0418 041a 0421 0410 0426 0418 042f 0418 041c 0418 0422 0418 0420 041e 0412 0410 041d 041d 042b 0425 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 042b 0421 041e 041a 041e 0419 0410 041a 0422 0418 0412 041d 041e 0421 0422 0418 0421 0422 0415 041a 041b 041e 041e 0411 0420 0410 0417 041d 042b 041c 0418 0422 0412 0415 0420 0414 042b 041c 0418 0412 0415 0429 0415 0421 0422 0412 0410 041c 0418 ; Fijacion de Desechos Simulados de Elevada Radiactividad en Solidos Vitreos

Abstract

Current laboratory development work at ORNL aims at incorporating high-activity-level wastes in high-density insoluble glasses, containing all radioactive constituents in the solid. Experiments with simulated TBP-25 (aluminium, HNOs), Purex and Darex (stainless steel, HNOs) wastes have indicated the technical feasibility of such a process. Dense, microcrystalline solids may be as acceptable as true glasses; their greater thermal conductivity compensates somewhat for the increase in surface area over that of true glasses. Phosphate and borophosphate glasses were prepared from all three types of waste in thelaboratory.Caesium volatility was limited to the - 0.1% due to physical entrainment, and ruthenium volatility was lowered to -0.5% by addition of phosphite or hypophosphite. Other additives included PbO, Ca(OH){sub 2}, NaOH, and MgO. Bulk densities varied from 2.36 to 2.90 g/cm{sup 3} for TBP-25 and from 2.63 to 2.80 g/cm{sup 3} for Purex waste. Corresponding volume reductions from the concentrated waste solutions were 7.2 -9.3 and 5.7 - 8.3; initial softening points varied from 875 to 100 Degree-Sign C and from 830 to 975 Degree-Sign C respectively. Darex tests are still preliminary. Semi-continuous operation on a semi-engineering scale produced a true glass from TBP-25 waste and a microcrystalline solid from Purex. The thermal conductivity of  More>>
Authors:
Clark, W. E.; Godbee, H. W. [1] 
  1. Oak Ridge National Laboratory, Oak Ridge, TN (United States)
Publication Date:
Feb 15, 1963
Product Type:
Conference
Resource Relation:
Conference: Symposium on Treatment and Storage of High-Level Radioactive Wastes Radioactive Wastes, Vienna (Austria), 8-12 Oct 1962; Other Information: 19 refs., 8 tabs., 10 figs.; Related Information: In: Treatment and Storage of High-Level Radioactive Wastes. Proceedings of the Symposium on Treatment and Storage of High-Level Radioactive Wastes| 686 p.
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; ACTIVITY LEVELS; BULK DENSITY; CALCINATION; CORROSION; ENGINEERING; EVAPORATION; GLASS; LIQUID WASTES; MAGNESIUM OXIDES; RADIOACTIVE WASTE DISPOSAL; RADIOACTIVE WASTE STORAGE; RADIOACTIVE WASTES; RUTHENIUM; SIMULATION; SODIUM HYDROXIDES; STAINLESS STEELS; SURFACE AREA; TBP; THERMAL CONDUCTIVITY; VOLATILITY
OSTI ID:
22182125
Research Organizations:
International Atomic Energy Agency, Vienna (Austria)
Country of Origin:
IAEA
Language:
English
Other Identifying Numbers:
Other: ISSN 0074-1884; TRN: XA13M3587006624
Submitting Site:
INIS
Size:
page(s) 411-439
Announcement Date:
Jan 23, 2014

Citation Formats

Clark, W. E., and Godbee, H. W. Fixation of Simulated Highly Radioactive Wastes in Glassy Solids; Fixation de Dechets Simules de Haute Activite dans des Soudes Vitreux; 0424 0418 041a 0421 0410 0426 0418 042f 0418 041c 0418 0422 0418 0420 041e 0412 0410 041d 041d 042b 0425 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 042b 0421 041e 041a 041e 0419 0410 041a 0422 0418 0412 041d 041e 0421 0422 0418 0421 0422 0415 041a 041b 041e 041e 0411 0420 0410 0417 041d 042b 041c 0418 0422 0412 0415 0420 0414 042b 041c 0418 0412 0415 0429 0415 0421 0422 0412 0410 041c 0418 ; Fijacion de Desechos Simulados de Elevada Radiactividad en Solidos Vitreos. IAEA: N. p., 1963. Web.
Clark, W. E., & Godbee, H. W. Fixation of Simulated Highly Radioactive Wastes in Glassy Solids; Fixation de Dechets Simules de Haute Activite dans des Soudes Vitreux; 0424 0418 041a 0421 0410 0426 0418 042f 0418 041c 0418 0422 0418 0420 041e 0412 0410 041d 041d 042b 0425 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 042b 0421 041e 041a 041e 0419 0410 041a 0422 0418 0412 041d 041e 0421 0422 0418 0421 0422 0415 041a 041b 041e 041e 0411 0420 0410 0417 041d 042b 041c 0418 0422 0412 0415 0420 0414 042b 041c 0418 0412 0415 0429 0415 0421 0422 0412 0410 041c 0418 ; Fijacion de Desechos Simulados de Elevada Radiactividad en Solidos Vitreos. IAEA.
Clark, W. E., and Godbee, H. W. 1963. "Fixation of Simulated Highly Radioactive Wastes in Glassy Solids; Fixation de Dechets Simules de Haute Activite dans des Soudes Vitreux; 0424 0418 041a 0421 0410 0426 0418 042f 0418 041c 0418 0422 0418 0420 041e 0412 0410 041d 041d 042b 0425 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 042b 0421 041e 041a 041e 0419 0410 041a 0422 0418 0412 041d 041e 0421 0422 0418 0421 0422 0415 041a 041b 041e 041e 0411 0420 0410 0417 041d 042b 041c 0418 0422 0412 0415 0420 0414 042b 041c 0418 0412 0415 0429 0415 0421 0422 0412 0410 041c 0418 ; Fijacion de Desechos Simulados de Elevada Radiactividad en Solidos Vitreos." IAEA.
@misc{etde_22182125,
title = {Fixation of Simulated Highly Radioactive Wastes in Glassy Solids; Fixation de Dechets Simules de Haute Activite dans des Soudes Vitreux; 0424 0418 041a 0421 0410 0426 0418 042f 0418 041c 0418 0422 0418 0420 041e 0412 0410 041d 041d 042b 0425 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 042b 0421 041e 041a 041e 0419 0410 041a 0422 0418 0412 041d 041e 0421 0422 0418 0421 0422 0415 041a 041b 041e 041e 0411 0420 0410 0417 041d 042b 041c 0418 0422 0412 0415 0420 0414 042b 041c 0418 0412 0415 0429 0415 0421 0422 0412 0410 041c 0418 ; Fijacion de Desechos Simulados de Elevada Radiactividad en Solidos Vitreos}
author = {Clark, W. E., and Godbee, H. W.}
abstractNote = {Current laboratory development work at ORNL aims at incorporating high-activity-level wastes in high-density insoluble glasses, containing all radioactive constituents in the solid. Experiments with simulated TBP-25 (aluminium, HNOs), Purex and Darex (stainless steel, HNOs) wastes have indicated the technical feasibility of such a process. Dense, microcrystalline solids may be as acceptable as true glasses; their greater thermal conductivity compensates somewhat for the increase in surface area over that of true glasses. Phosphate and borophosphate glasses were prepared from all three types of waste in thelaboratory.Caesium volatility was limited to the - 0.1% due to physical entrainment, and ruthenium volatility was lowered to -0.5% by addition of phosphite or hypophosphite. Other additives included PbO, Ca(OH){sub 2}, NaOH, and MgO. Bulk densities varied from 2.36 to 2.90 g/cm{sup 3} for TBP-25 and from 2.63 to 2.80 g/cm{sup 3} for Purex waste. Corresponding volume reductions from the concentrated waste solutions were 7.2 -9.3 and 5.7 - 8.3; initial softening points varied from 875 to 100 Degree-Sign C and from 830 to 975 Degree-Sign C respectively. Darex tests are still preliminary. Semi-continuous operation on a semi-engineering scale produced a true glass from TBP-25 waste and a microcrystalline solid from Purex. The thermal conductivity of the glass varied from 1.05 BTU/hr-ft-F Degree-Sign at 320 Degree-Sign F to 1.6 at 1050 Degree-Sign F, about 10 times higher than that of the calcine without additives. Ruthenium volatility was held to <10% by phosphite addition. Stainless steel is a satisfactory material for construction of the calcination-fixation container. Essentially all the internal corrosion takes place during the relatively short (2-6 hr) period in which the last of the acid and water are expelled at the maximum temperature. Melt production increased the corrosion of 304L stainless steel from 5 to 42 mil/month for a 24-hr evaporation-fixation cycle on TBP-25 waste and from 8 to 140 mil/ month on Purex waste. Operation above 900 Degree-Sign C with Purex waste plus fluxing agents may result in catastrophic local corrosion. (author) [French] Le Laboratoire national d'Oak Ridge s'efforce actuellement de mettre au point un methode d'incorporation des dechets de haute activite dans des verres insolubles de densite elevee, tous les elements radioactifs se trouvant contenus dans la partie solide. Des experiences avec des dechets simules resultant des procedes TBP-25 (aluminium, HNO{sub 3}), Purex et Darex (acier inoxydable, HNO{sub 3}) montrent qu'une telle methode est techniquement realisable. Des solides denses, de structure microcristalline, peuvent convenir aussi bien que de veritables, verres; leur meilleure conductibilite thermique compense dans une certaine mesure le fait que la surface doit etre plus grande que dans le cas des verres. Avec les types de dechets susmentionnes, on a prepare des verres au phosphate et au borophosphate. La volatilite du cesium etait limitee a 0,1% environ du fait de l'entrainement mecanique et la volatilite du ruthenium a ete abaissee a moins de 0,5% par addition de phosphite ou d'hypophosphite. Parmi les autres additifs figuraient PbO, Ca(OH){sub 2}, NaOH et MgO. Les densites brutes variaient entre 2,36 et 2,90 g/cm{sup 3} pour les dechets du procede TBP-25 et entre 2,63 et 2,80 g/cms pour les dechets du procede Purex. Les reductions de volume correspondantes, a partir des solutions concentrees de dechets, etaient comprises entre 7,2 et 9,3 et entre 5,7 et 8,3; le passage initial a l'etat pateux se produisait entre 875 et 1000 Degree-Sign C et entre 830 et 975 Degree-Sign C respectivement. Les essais avec les dechets Darex en sont encore au stade preliminaire. En operant de maniere semi-continue a l'echelle semi-industrielle' on a obtenu un verre veritable a partir de dechets TBP-25 et un solide microcristallin a partir de dechets Purex. La conductibilite thermique du verre variait entre 5,07 W/cm. Degree-Sign C a 160 Degree-Sign C et 7,73 W/cm. Degree-Sign C a 565 Degree-Sign C, c'est-a-dire qu'elle est 10 fois superieure a celle de la masse calcinee sans additifs. La volatilite du ruthenium a ete maintenue a moins de 10% par addition de phosphite. Le recipient de calcination-fixation peut etre construit en acier inoxydable. Pratiquement toute la corrosion interne se produit au cours de la periode relativement breve (2 a 6 h) au cours de laquelle les derniers residus d'acier et d'eau sont chasses a la temperature maximum. La formation de verre fondu a augmente la corrosion de l'acier inoxydable 304L de 0,12 a 1,05 mm par mois, pour un cycle d'evaporation-fixation de 24 heures, dans le cas des dechets du procede TBP-25 et de 0,20 a 3,5 mm par mois dans celui des dechets Purex. Si l'on travaille a plus de 900 Degree-Sign C sur des dechets Purex en presence de fondants, une corrosion localisee extremement grave risque de se produire. (author) [Spanish] En el Oak Ridge National Laboratory se procura perfeccionar metodos para incorporar desechos de elevada radiactividad a vidrios insolubles de gran densidad, que contengan todos los componentes radiactivos en la fraccion solida. Los experimentos con desechos simulados de los procesos TBP-25 (aluminio, HNO{sub 3}), Purex y Darex (acero inoxidable, HNOj) demuestran que tales metodos son tecnicamente factibles. Los solidos densos, de estructura nucrocristalina pueden ser tan aceptables como los vidrios verdaderos; su mayor conductividad termica compensa hasta cierto punto el aumento de superficie con respecto a la de los vidrios verdaderos. Con los mencionados tipos de desechos se prepararon en el laboratorio vidrios al fosfato y al borofosfato. La volatilidad del cesio se limito al 0,1 por ciento, aproximadamente, debido al arrastre mecanico y la volatilidad del rutenio se rebajo a menos de 0,5%, agregando fosfito o hipofosfito a la mezcla. Entre los otros aditivos figuran el PbO, el Ca(OH){sub 2}, el NaOH, y el MgO. Las densidades brutas varian entre 2,36 y 2,90 g/cm{sup 3} para los desechos del proceso TBP-25 y entre 2,63 y 2,80 g/cm{sup 3} para los del Purex. Las reducciones de volumen correspondientes a las soluciones concentradas de desechos estan comprendidas entre 7,2 y 9,3 y entre 5,7 y 8,3; los puntos de reblandecimiento iniciales varian entre 875 y 1000 Degree-Sign C y entre 830 y 975 Degree-Sign C, respectivamente. Los ensayos con los desechos Darex se encuentran aun en la etapa preliminar. Al trabajar de manera semicontinua, en escala semiindustrial, se obtuvo un vidrio verdadero partiendo de desechos TBP-25 y un solido microcristalino partiendo de desechos Purex. La conductividad termica del vidrio varfa entre 1,05 BTU/h pie 'F a 320 Degree-Sign F y 1,6 a 1050 Degree-Sign F, es decir, que es 10 veces superior a la de la masa calcinada sin aditivos. La volatilidad del rutenio se mantuvo por debajo del 10% anadiendo fosfito. El acero inoxidable constituye un material satisfactorio para la construccion del recipiente de calcinacion- fijacion. Practicamente toda la corrosion interna se produce durante el periodo relativamente breve (2 a 6 h) en el que se expulsan los ultimos residuos de acido y agua a la temperatura maxima. La formacion de vidrio fundido acrecento la corrosion del acero inoxidable 304L de 5 a 42 milesimas de pulg/mes, en un ciclo de evaporacion-fijacion de 24 horas, en el caso de los desechos del proceso TBP-25 y de 8 a 140 milesimas de pulg/mes, en el de los desechos Purex. Al trabajar a mas de 900 Degree-Sign C con desechos Purex y fundentes anadidos, puede originarse una corrosion localizada sumamente seria. (author) [Russian] Cel'ju novyh rabot v Okriohskoj nacional'noj laboratorii, javljaetsja vkljuchenie radioaktivnyh othodov vysokoj aktivnosti v nerastvorimye stekla s vysokoj plotnost'ju, uderzhivajushhie voe radioaktivnye veshhestva v tverdom sostojanii. Jeksperimenty s imitirovannymi othodami ''TBF-25-processa'', ''Pureks-processa'' (aljuminij, HNO{sub 3}) i ''Dareks-processa'' (nerzhavejushhaja stal', HNOa) pokazali tehnologicheskuju vypolnimost' takogo processa. Plotnye mikrokristallicheskie tverdye veshhestva mogut byt' stol' zhe priemlemymi, kak istinnye stekla; ih bol'shaja teploprovodnost' v nekotoroj mere vozmeshhaet uvelichenie poverhnosti po sravneniju s istinnymi steklami. V laboratorii byli izgotovleny fosfatnye i borfosfatnye stekla iz othodov vseh jetih treh vidov. Letuchest' cezija byla ogranichena do -v0,1% za schet fizicheskogo uvlechenija, a letuchest' rutenija byla snizhena do <0,3% dobavleniem fosfita i gipofosfita. Drugimi dobavochnymi veshhestvami sluzhili: PbO, Ca (OH){sub 2}, NaOH i MgO. Udel'nyj ves massy izmenjalsja ot 2,36 do 2,90 g/cm{sup 3} dlja othodov 'TBF-25-processa' i ot 2,63 do 2,60 g/smje dlja othodov {sup P}ureks-processa{sup .} Ob{sup e}m umenyvaloja po sravneniju s ishodnymi ob{sup e}mami koncentrirovannyh rastvorov othodov v pervom sluchae v 7,2 - 9,3 raza i vo vtorom sluchae v 5,7 - 8,3 raza; tochki nachal'nogo razmjagchenija izmenjalis' sootvetstvenno ot 675 do 1 000 Degree-Sign C i ot 830 do 975vS. Rezul'taty opytov o othodami 'Dareks-processa' vse eshhe nosjat predvaritel'nyj harakter. V rezul'tate polunepreryvnogo processa v poluproizvodstvennom masshtabe poluchalis' istinnye stekla iz othodov ''TBF-25-processa'' i mikrokristallicheskoe tverdoe veshhestvo iz othodov {sup P}ureks- processa{sup .} Teploprovodnost' stekla izmenjalas' ot 1,05 britanskih termicheskih edinic v chas na fu*g i na 1 Degree-Sign F pri 320 Degree-Sign F do 1,6 pri 1 050 Degree-Sign F, t.e. ona v 10 raz prevyshala teploprovodnost' obzhigaemogo veshhestva bez dobavok. Blagodarja dobavleniju fosfita letuchest' rutenija snizhalas' do <10%. Nerzhavejushhaja stal' javljaetsja udovletvoritel'nym materialom dlja izgotovlenija kontejnerov dlja obzhiganija i fiksacii. Pochti vsja vnutrennjaja korrozija proishodit v techenie otnositel'no korotkogo perioda vremeni (2-6 chasov), v techenie kotorogo pri maksimal'noj temperature udaljajutsja poslednie ostatki kislot i vody. Obrazovanie rasplavlennoj massy uvelichivaet korroziju nerzhavejushhej stali sorta 304L s 5 do 42 tysjachnyh djujma v mesjah dlja 24-chasovogo cikla uparivanija i fiksacii dlja othodov ''TBF-25-processa'' i s 8 do 140 tysjachnyh djujma v mesjac dlja othoda, ''Pureks-processa''. Rabota pri temperature svyshe 900 Degree-Sign C s othodami 'Pureks-processa' i s dobavleniem fljusov mozhet privesti k katastroficheskoj mestnoj korrozii. (author)}
place = {IAEA}
year = {1963}
month = {Feb}
}