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Calcination of Radioactive Waste in Molten Sulphur; Calcination de Dechets Radioactifs dans le Soufre Fondu; 041a 0410 041b 042c 0426 0418 041d 0418 0420 041e 0412 0410 041d 0418 0415 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 0420 0410 0421 041f 041b 0410 0412 041b 0415 041d 041d 041e 0419 0421 0415 0420 0415 ; Calcinacion de Desechos Radiactivos en Azufre Fundido

Conference:

Abstract

The Savannah River Laboratory is developing a novel process based on the unique properties of sulphur for converting radioactive wastes to a solid form of low solubility for ''ultimate'' disposal. In this process the aqueous acidic wastes are reacted with molten sulphur at 150 Degree-Sign C so that the water and volatile acids are driven off and the chemical compounds present in the waste are calcined and/or chemically reduced. The resulting sulphur-waste slurry is then heated at 400 to 444 Degree-Sign C for from 1 to 5 hr to drive off sulphuric acid and residual water and further calcine and/or reduce the chemical compounds in the sulphur-waste slurry. In these steps the molten sulphur serves as a heat-transfer medium, prevents the entrainment of the radioactive solids in the steam and reaction gases and eliminates the volatilization of radioactive ruthenium by preventing the formation of the tetroxide. Laboratory scale runs with concentrated high activity waste as feed (1.3 x 10{sup 9} {gamma} c/(min)(ml), 2.0M Al(N0{sub 3}){sub 3}, and 1.5M HNO{sub 3}) have shown that only one part in approximately 100 000 parts of the activity in the feed is carried overhead in the off-gas in these process steps. After the completion  More>>
Authors:
Winsche, W. E.; Davis, Jr., M. W.; Goodlett, Jr., C. B.; Occhipinti, E. S.; Webster, D. S. [1] 
  1. E.I. Du Pont de Nemours and Co., Aiken, SC (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: 13 refs., 7 figs., 5 tabs.; 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; ALUMINIUM NITRATES; CALCINATION; CONTAINMENT SYSTEMS; EVAPORATION; HEAT TRANSFER; HIGH-LEVEL RADIOACTIVE WASTES; NITRIC ACID; RADIOACTIVE WASTE DISPOSAL; RADIOACTIVE WASTE PROCESSING; RADIOACTIVE WASTE STORAGE; RUTHENIUM; SAVANNAH RIVER; SLURRIES; STAINLESS STEELS; SULFUR; SULFURIC ACID
OSTI ID:
22182116
Research Organizations:
International Atomic Energy Agency, Vienna (Austria)
Country of Origin:
IAEA
Language:
English
Other Identifying Numbers:
Other: ISSN 0074-1884; TRN: XA13M3577006615
Submitting Site:
INIS
Size:
page(s) 195-215
Announcement Date:
Jan 23, 2014

Conference:

Citation Formats

Winsche, W. E., Davis, Jr., M. W., Goodlett, Jr., C. B., Occhipinti, E. S., and Webster, D. S. Calcination of Radioactive Waste in Molten Sulphur; Calcination de Dechets Radioactifs dans le Soufre Fondu; 041a 0410 041b 042c 0426 0418 041d 0418 0420 041e 0412 0410 041d 0418 0415 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 0420 0410 0421 041f 041b 0410 0412 041b 0415 041d 041d 041e 0419 0421 0415 0420 0415 ; Calcinacion de Desechos Radiactivos en Azufre Fundido. IAEA: N. p., 1963. Web.
Winsche, W. E., Davis, Jr., M. W., Goodlett, Jr., C. B., Occhipinti, E. S., & Webster, D. S. Calcination of Radioactive Waste in Molten Sulphur; Calcination de Dechets Radioactifs dans le Soufre Fondu; 041a 0410 041b 042c 0426 0418 041d 0418 0420 041e 0412 0410 041d 0418 0415 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 0420 0410 0421 041f 041b 0410 0412 041b 0415 041d 041d 041e 0419 0421 0415 0420 0415 ; Calcinacion de Desechos Radiactivos en Azufre Fundido. IAEA.
Winsche, W. E., Davis, Jr., M. W., Goodlett, Jr., C. B., Occhipinti, E. S., and Webster, D. S. 1963. "Calcination of Radioactive Waste in Molten Sulphur; Calcination de Dechets Radioactifs dans le Soufre Fondu; 041a 0410 041b 042c 0426 0418 041d 0418 0420 041e 0412 0410 041d 0418 0415 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 0420 0410 0421 041f 041b 0410 0412 041b 0415 041d 041d 041e 0419 0421 0415 0420 0415 ; Calcinacion de Desechos Radiactivos en Azufre Fundido." IAEA.
@misc{etde_22182116,
title = {Calcination of Radioactive Waste in Molten Sulphur; Calcination de Dechets Radioactifs dans le Soufre Fondu; 041a 0410 041b 042c 0426 0418 041d 0418 0420 041e 0412 0410 041d 0418 0415 0420 0410 0414 0418 041e 0410 041a 0422 0418 0412 041d 042b 0425 041e 0422 0425 041e 0414 041e 0412 0412 0420 0410 0421 041f 041b 0410 0412 041b 0415 041d 041d 041e 0419 0421 0415 0420 0415 ; Calcinacion de Desechos Radiactivos en Azufre Fundido}
author = {Winsche, W. E., Davis, Jr., M. W., Goodlett, Jr., C. B., Occhipinti, E. S., and Webster, D. S.}
abstractNote = {The Savannah River Laboratory is developing a novel process based on the unique properties of sulphur for converting radioactive wastes to a solid form of low solubility for ''ultimate'' disposal. In this process the aqueous acidic wastes are reacted with molten sulphur at 150 Degree-Sign C so that the water and volatile acids are driven off and the chemical compounds present in the waste are calcined and/or chemically reduced. The resulting sulphur-waste slurry is then heated at 400 to 444 Degree-Sign C for from 1 to 5 hr to drive off sulphuric acid and residual water and further calcine and/or reduce the chemical compounds in the sulphur-waste slurry. In these steps the molten sulphur serves as a heat-transfer medium, prevents the entrainment of the radioactive solids in the steam and reaction gases and eliminates the volatilization of radioactive ruthenium by preventing the formation of the tetroxide. Laboratory scale runs with concentrated high activity waste as feed (1.3 x 10{sup 9} {gamma} c/(min)(ml), 2.0M Al(N0{sub 3}){sub 3}, and 1.5M HNO{sub 3}) have shown that only one part in approximately 100 000 parts of the activity in the feed is carried overhead in the off-gas in these process steps. After the completion of the high-temperature treatment, the sulphur-waste slurry is cooled to 120-150 Degree-Sign C and transferred as a liquid to the final containment system where it is allowed to solidify. Although it is our intent to protect the containment system against the action of water, the resistance of the solidified sulphur- waste slurry to the action of water has been used as a measure of the effectiveness of this process. Small cylinders of the solidified slurry have been prepared from simulated wastes containing Al (NO{sub 3}){sub 3} or dissolved stainless-steel nitrates with tracer levels of Sr and Cs, and for concentrated high-activity waste containing Al(NO{sub 3}s){sub 3}. These cylinders have been exposed to water over extended periods of time. Leaching rates are calculated as, though there is complete removal of material from a surface layer. Rates of 10 to 20 mil/yr, or less, have been observed after an initial period of 6 to 8 weeks at moderately higher rates. (author) [French] Le Laboratoire de Savannah River met actuellement au point une methode nouvelle fondee sur les proprietes exceptionnelles du soufre qui permettent de transformer des dechets radioactifs en solides peu solubles, en vue de proceder a leur elimination definitive. Selon cette methode, on fait reagir les dechets liquides acides avec du soufre fondu a 150 Degree-Sign C: l'eau et les acides volatiles sont chasses, puis les composes chimiques presents dans les dechets sont calcines et/ou reduits chimiquement. La suspension soufre-dechets ainsi obtenue est alors chauffee pendant une duree de 1 a 5h aune temperature de 400 a 444 Degree-Sign C afin de chasser l'acide sulfurique et l'eau residuelle et de poursuivre la calcination et/ou la reduction des composes chimiques dans la suspension soufre-dechets. Au cour de ces operations, ie soufre fondu sert de milieu caloporteur, empeche l'entrainement des solides radioactifs dans la vapeur et les gaz de la reaction et previent la volatilisation du radioruthenium en empechant la formation du tetraoxyde. Des essais en laboratoire avec des dechets concentres de haute activite (1.3 x 10{sup 9} {gamma} c/(min)(ml), 2.0M Al(N0{sub 3}){sub 3}, et 1.5M HNO{sub 3}) ont montre qu'environ un cent-millieme seulement de l'activite presente dans la matiere premiere est emporte par le gaz qui se degage au cours de ces operations. Une fois termine le traitement a haute temperature, on laisse refroidir la suspension soufre-dechets jusqu'a 150 ou 120 Degree-Sign C et on la transvase ensuite dans le milieu d'isolement final, ou on la laisse se solidifier. Bien que les auteurs aient l'intention de proteger le milieu d'isolement contre l'action de l'eau, ils ont etudie la resistance de la suspension solidifiee soufre-dechets a l'action de l'eau pour verifier l'efficacite du procede. On a fabrique de petits cylindres de la suspension solidifiee obtenue a partir de dechets simules qui contenaient Al(NO{sub 3}){sub 3} sou de nitrates formes par dissolution de l'acier inoxydable, avec des traces de Sr et Cs, ainsi que de dechets concentres de haute activite qui contenaient Al(NO{sub 3}){sub 3}. Ces cylindres ont ete exposes a l'action de l'eau pendant de longues periodes. On a calcule les vitesses de lixiviation comme s'il y avait elimination complete de matiere sur une couche superficielle. Les vitesses enregistrees correspondent a des valeurs de 0,25 a 0,50 mm par an, au plus, apres une periode initiale de six a huit semaines durant laquelle on a enregistre des vitesses legerement superieures. (author) [Spanish] En el Savannah River Laboratory se esta perfeccionando un nuevo procedimiento basado en las peculiares propiedades del azufre que permiten transformar los desechos radiactivos en solidos de baja solubilidad, aptos para una evacuacion ''definitiva''. Segun dicho procedimiento, los desechos acuosos acidos se hacen reaccionar con azufre fundido a 150 Degree-Sign C lo cual se expulsa el agua y los acidos volatiles, mientras que los compuestos quimicos presentes en los desechos quedan calcinados, y/o quimicamente reducidos. La suspension azufre-desechos asi formada se calienta entonces entre 400 Degree-Sign y 444 Degree-Sign C, durante 1 a 5 h, para expulsar el acido sulfuricoy el agua residual y los compuestos quimicos se vuelven a calcinar o a reducir, o ambas cosas a la vez, segun convenga, en la suspension azufre-desechos. En estas operaciones, el azufre fundido actua como medio de transmision del calor, impide el arrastre de solidos radiactivos en el vapor y los gases de la reaccion y suprime la volatilizacion del rutenio radiactivo, al impedir la formacion del tetraoxido respectivo. Los ensayos de laboratorio efectuados con desechos de elevada radiactividad (1.3 x 10{sup 9} {gamma} c/(min)(ml), 2.0M Al(NO{sub 3}){sub 3}, 1.5M HNO{sub 3}) han demostrado que tan solo una cienmilesima parte, aproximadamente, de la actividad presente en la carga es arrastrada por el gas desprendido en estas operaciones. Una vez terminado el tratamiento a alta temperatura,la suspension azufre-desechos se enfria hasta 120 o 150 Degree-Sign C y se transporta en forma de liquido al sistema de confinamiento final, donde se la deja solidificar. Aunque los autores tienen el proposito de proteger el sistema de confinamiento contra la accion del agua, han utilizado la resistencia de la suspension solidificada azufre-desechos a la accion del agua como medida de la eficacia del procedimiento. Se prepararon pequenos cilindros de suspension solidificada de desechos simulados que contenian Al(NO{sub 3}){sub 3}, o los nitratos formados disolviendo acero inoxidable, con vestigios de Sr y Cs, asi como de desechos concentrados de elevada actividad que contenian Al(NO{sub 3}){sub 3}. Estos cilindros se expusieron a la accion del agua durante periodos prolongados. Se calculan las velocidades de lixiviacion como si se eliminara totalmente el material de una capa superficial. Las velocidades registradas oscilan entre 10 y 20 milesimas de pulg/anio,o menos, despues de un periodo inicial de 6 a 8 semanas durante el cual adoptan valores algo mas elevados. (author) [Russian] Laboratorija Savanna River razrabatyvaet metod prevrashhenija radioaktivnyh othodov v tverdyj produkt s maloj rastvorimost'ju dlja 'okonchatel'nogo' ih udalenija. Novyj metod osnovan na iskljuchitel'nyh svojstvah sery. V jetom processe kislye vodnye othody podvergajutsja vozdejstviju rasplavlennoj sery pri 150 Degree-Sign C, chto vedet k ispareniju vody i letuchih kislot, posle chego soderzhashhiesja v othodah himicheskie soedinenija kal'cinirujutsja i vosstanavlivajutsja himicheskim sposobom. Poluchapciesja v vide sernogo shlamma othody nagrevajutsja pri temperature 400 Degree-Sign - 444 Degree-Sign C v techenie odnogo - pjati chasov dlja udalenija sernoj kisloty i ostavshejsja vody i dlja dal'nejshego kvl'ninirovanija i vosstanovlenija himicheskih soedinenij v sbrosnom sernom shlamme. Na jetih stadijah rasplavlennaja sera sluzhit v kachestve teploprovodnoj sredy, prepjatstvuet uvlecheniju radioaktivnyh tverdyh chastic obrazujushhimisja parami i gazami, a takzhe uletuchivaniju radioaktivnogo rutenija ne dopuskaja obrazovanija chetyrehokiela. Laboratornye opyty s ispol'zovaniem v kachestve pitajushhego rastvora koncentrirovannyh othodov vysokoj aktivnosti (1.3 x 10{sup 9} {gamma} c/(min)(ml), 2.0M Al(N0{sub 3}){sub 3}, i 1.5M HNO{sub 3}) pokazali, chto na jetih stadijah processa vyhodjashhimi gazami uvlekaetsja priblizitel'no lish' odna chast' na 100 000 chastej aktivnosti, soderzhashhejsja v ishodnom produkte. Po okonchanii vysokotemperaturnoj obrabotki sbrosnoj sernyj shlamm ohlazhdaetsja do 120 Degree-Sign C - 150 Degree-Sign C i slivaetsja v emkosti dlja okonchatel'nogo hranenija, v kotoryh on zatverdevaet. Stojkost' zatverdevshego sbrosnogo sernogo olamma protiv vozdejstvija vody byla ispol'zovana v kachestve mery jeffektivnosti jetogo metoda obrabotki, hotja avtory ne otkazyvajutsja ot zashhity sistemy emkostej protiv vozdejstvija vody. Iz imitirujushhih rastvorov, soderzhashhih Al(NO{sub 3}){sub 3} jeili nitraty rastvorennoj nerzhavejushhej stali s indikatornymi kolichestvami radioaktivnogo stroncija i cezija, a takzhe iz koncentrirovannyh vysokoradioaktivnyh othodov, soderzhashhih Al(NO{sub 3}){sub 3}, byli izgotovleny nebol'shie cilindry otverzhdennogo shlamma. Jeti cilindry podvergalis' dlitel'nomu vozdejstviju vody. Skorost' vyshhelachivanija opredeljalas' iz rascheta polnogo udalenija materiala iz poverhnostnogo sloja. Posle pervonachal'nogo perioda (6-8 nedel'), kogda vyshhelachivanie proishodit sravnitel'no bystro, nabljudaemaja skorost' vyshhelachivanija sostavljala 0,25 - 0,50 mm v god. (author)}
place = {IAEA}
year = {1963}
month = {Feb}
}