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Title: Iron Phosphate Glass for Vitrifying Hanford AZ102 LAW in Joule Heated and Cold Crucible Induction Melters - 12240

Abstract

An iron phosphate composition for vitrifying a high sulfate (∼17 wt%) and high alkali (∼80 wt%) Hanford low activity waste (LAW), known as AZ-102 LAW, has been developed for processing in a Joule Heated Melter (JHM) or a Cold Crucible Induction Melter (CCIM). This composition produced a glass waste form, designated as MS26AZ102F-2, with a waste loading of 26 wt% of the AZ-102 which corresponded to a total alkali and sulfate (represented as SO{sub 3}) content of 21 and 4.4 wt%, respectively. A slurry (7 M Na{sup +}) of MS26AZ102F-2 simulant was melted continuously at temperatures between 1030 and 1090 deg. C for 10 days in a small JHM at PNNL and for 70 hours in a CCIM at INL. The as-cast glasses produced in both melters and in trial laboratory experiments along with their canister centerline cooled (CCC) counterparts met the requirements for the Product Consistency Test (PCT) and the Vapor Hydration Test (VHT) responses in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) Contract. These glass waste forms retained up to 77 % of the SO{sub 3} (3.3 wt%), 100% of the Cesium, and 33 to 44% of the rhenium (used as a surrogate for Tc) allmore » of which either exceeded or were comparable to the retention limit for these species in borosilicate glass nuclear waste form. Analyses of commercial K-3 refractory lining and the Inconel 693 metal electrodes used in JHM indicated only minimum corrosion of these components by the iron phosphate glass. This is the first time that an iron phosphate composition was melted continuously in a slurry fed JHM and in the US, thereby, demonstrating that iron phosphate glasses can be used as alternative hosts for vitrifying nuclear waste. The following conclusions are drawn from the results of the present work. (1) An iron phosphate composition, designated as MS26AZ102F-2, containing 26 wt% of the simulated high sulfate (17 wt%), high alkali (80 wt%) Hanford AZ-102 LAW meets all the criteria for processing in a JHM and CCIM. This composition produces a homogeneous glass with a density of 2.80 ± 0.04 g/cm{sup 3} after melting between 1000 and 1050 deg. C for 3 to 5 h. (2) This is the first time that an iron phosphate glass was melted in the JHM continuously for 10 days achieving a specific melting rate of 1010 kg/m2/day and in the CCIM for 70 hrs with a melting rate of 664 kg/m{sup 2}/day. (3) The analyzed (ICP-AES) compositions for all the glasses prepared under several melting conditions are in excellent agreement with the target composition. The variation of melting conditions include: (i) use of small scale/short melting time to large scale/long melting time (300 g to 80 kg, 4 h to 10 days) operations including melting in the JHM and CCIM, (ii) use of dry or wet (slurry) melter feed, (iii) addition of reductant (sugar) in the batch, and (iv) bubbling the melt with air. (4) The chemical durability as measured by PCT and VHT for the quenched and CCC-treated waste forms prepared from laboratory, JHM or CCIM melting exceeds the DOE requirements for LAW. (5) Depending upon the melting time (4 h to 10 days), the average concentration of SO{sub 3} in the MS26AZ102F-2 iron phosphate glass waste form varies from about 1.78 (RSM) to 3.74 (laboratory melt) wt% which corresponds to an SO{sub 3} retention of 41 to 86% when melted between 1030 at 1050 deg. C in air. (6) The retention of SO{sub 3} in the glass was reduced when a reductant (sugar) was added to the slurry. (7) The retention of other problem components like Cesium and Rhenium/Tc-99 is also high; from 92 to 100% for Cs{sub 2}O under different melting conditions, and from 66 to 33% for Re{sub 2}O{sub 7} for melts processed from 3 to 5 hours and up to 10 days. (8) Corrosion tests on Inconel 693 and K-3 refractory at temperatures between 1000 and 1050 deg. C indicate that both materials should be suitable for melting iron phosphate glasses. (9) The viscosity and electrical conductivity of the MS26AZ102F-2 melt are within the acceptable limits for RSM and CCIM processing. (10)This work has shown that iron phosphate compositions are a potential alternative to borosilicate glasses for vitrifying problematic wastes such as Hanford AZ-102 LAW that contains high amounts sulfate and alkali oxides, and that iron phosphate melts such as MS26AZ102F-2 can be processed in the JHM or CCIM. (authors)« less

Authors:
; ; ;  [1];  [2]; ;  [3]; ; ;  [4];  [5]; ;  [6]
  1. Missouri University of Science and Technology, 1870 Miner Circle, Rolla, MO 65409 (United States)
  2. MO-SCI Corporation, 4040 HyPoint North, Rolla, MO 65401 (United States)
  3. Pacific North West National Laboratory, Battelle Blvd., Richland, WA 99352 (United States)
  4. Savannah River National Laboratory, Savannah River Site, 999-W, Aiken, SC 29803 (United States)
  5. Idaho National Laboratory, 2525 Fremont Avenue, Idaho Falls, ID 83415 (United States)
  6. Catholic University of America, 620 Michigan Avenue, N.E., Washington, DC 20064 (United States)
Publication Date:
Research Org.:
WM Symposia, 1628 E. Southern Avenue, Suite 9-332, Tempe, AZ 85282 (United States)
OSTI Identifier:
22293528
Report Number(s):
INIS-US-14-WM-12240
TRN: US14V1183115052
Resource Type:
Conference
Resource Relation:
Conference: WM2012: Waste Management 2012 conference on improving the future in waste management, Phoenix, AZ (United States), 26 Feb - 1 Mar 2012; Other Information: Country of input: France; 21 refs.
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; AUGER ELECTRON SPECTROSCOPY; BOROSILICATE GLASS; CESIUM; CESIUM OXIDES; IRON PHOSPHATES; MELTING; RETENTION; RHENIUM; SACCHAROSE; SULFATES; SULFITES; TECHNETIUM 99; WASTE FORMS; WASTE PROCESSING

Citation Formats

Day, Delbert E., Brow, Richard K., Ray, Chandra S., Reis, Signo T., Kim, Cheol-Woon, Vienna, John D., Sevigny, Gary, Peeler, David, Johnson, Fabienne C., Hansen, Eric K., Soelberg, Nick, Pegg, Ian L., and Gan, Hao. Iron Phosphate Glass for Vitrifying Hanford AZ102 LAW in Joule Heated and Cold Crucible Induction Melters - 12240. United States: N. p., 2012. Web.
Day, Delbert E., Brow, Richard K., Ray, Chandra S., Reis, Signo T., Kim, Cheol-Woon, Vienna, John D., Sevigny, Gary, Peeler, David, Johnson, Fabienne C., Hansen, Eric K., Soelberg, Nick, Pegg, Ian L., & Gan, Hao. Iron Phosphate Glass for Vitrifying Hanford AZ102 LAW in Joule Heated and Cold Crucible Induction Melters - 12240. United States.
Day, Delbert E., Brow, Richard K., Ray, Chandra S., Reis, Signo T., Kim, Cheol-Woon, Vienna, John D., Sevigny, Gary, Peeler, David, Johnson, Fabienne C., Hansen, Eric K., Soelberg, Nick, Pegg, Ian L., and Gan, Hao. Sun . "Iron Phosphate Glass for Vitrifying Hanford AZ102 LAW in Joule Heated and Cold Crucible Induction Melters - 12240". United States.
@article{osti_22293528,
title = {Iron Phosphate Glass for Vitrifying Hanford AZ102 LAW in Joule Heated and Cold Crucible Induction Melters - 12240},
author = {Day, Delbert E. and Brow, Richard K. and Ray, Chandra S. and Reis, Signo T. and Kim, Cheol-Woon and Vienna, John D. and Sevigny, Gary and Peeler, David and Johnson, Fabienne C. and Hansen, Eric K. and Soelberg, Nick and Pegg, Ian L. and Gan, Hao},
abstractNote = {An iron phosphate composition for vitrifying a high sulfate (∼17 wt%) and high alkali (∼80 wt%) Hanford low activity waste (LAW), known as AZ-102 LAW, has been developed for processing in a Joule Heated Melter (JHM) or a Cold Crucible Induction Melter (CCIM). This composition produced a glass waste form, designated as MS26AZ102F-2, with a waste loading of 26 wt% of the AZ-102 which corresponded to a total alkali and sulfate (represented as SO{sub 3}) content of 21 and 4.4 wt%, respectively. A slurry (7 M Na{sup +}) of MS26AZ102F-2 simulant was melted continuously at temperatures between 1030 and 1090 deg. C for 10 days in a small JHM at PNNL and for 70 hours in a CCIM at INL. The as-cast glasses produced in both melters and in trial laboratory experiments along with their canister centerline cooled (CCC) counterparts met the requirements for the Product Consistency Test (PCT) and the Vapor Hydration Test (VHT) responses in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) Contract. These glass waste forms retained up to 77 % of the SO{sub 3} (3.3 wt%), 100% of the Cesium, and 33 to 44% of the rhenium (used as a surrogate for Tc) all of which either exceeded or were comparable to the retention limit for these species in borosilicate glass nuclear waste form. Analyses of commercial K-3 refractory lining and the Inconel 693 metal electrodes used in JHM indicated only minimum corrosion of these components by the iron phosphate glass. This is the first time that an iron phosphate composition was melted continuously in a slurry fed JHM and in the US, thereby, demonstrating that iron phosphate glasses can be used as alternative hosts for vitrifying nuclear waste. The following conclusions are drawn from the results of the present work. (1) An iron phosphate composition, designated as MS26AZ102F-2, containing 26 wt% of the simulated high sulfate (17 wt%), high alkali (80 wt%) Hanford AZ-102 LAW meets all the criteria for processing in a JHM and CCIM. This composition produces a homogeneous glass with a density of 2.80 ± 0.04 g/cm{sup 3} after melting between 1000 and 1050 deg. C for 3 to 5 h. (2) This is the first time that an iron phosphate glass was melted in the JHM continuously for 10 days achieving a specific melting rate of 1010 kg/m2/day and in the CCIM for 70 hrs with a melting rate of 664 kg/m{sup 2}/day. (3) The analyzed (ICP-AES) compositions for all the glasses prepared under several melting conditions are in excellent agreement with the target composition. The variation of melting conditions include: (i) use of small scale/short melting time to large scale/long melting time (300 g to 80 kg, 4 h to 10 days) operations including melting in the JHM and CCIM, (ii) use of dry or wet (slurry) melter feed, (iii) addition of reductant (sugar) in the batch, and (iv) bubbling the melt with air. (4) The chemical durability as measured by PCT and VHT for the quenched and CCC-treated waste forms prepared from laboratory, JHM or CCIM melting exceeds the DOE requirements for LAW. (5) Depending upon the melting time (4 h to 10 days), the average concentration of SO{sub 3} in the MS26AZ102F-2 iron phosphate glass waste form varies from about 1.78 (RSM) to 3.74 (laboratory melt) wt% which corresponds to an SO{sub 3} retention of 41 to 86% when melted between 1030 at 1050 deg. C in air. (6) The retention of SO{sub 3} in the glass was reduced when a reductant (sugar) was added to the slurry. (7) The retention of other problem components like Cesium and Rhenium/Tc-99 is also high; from 92 to 100% for Cs{sub 2}O under different melting conditions, and from 66 to 33% for Re{sub 2}O{sub 7} for melts processed from 3 to 5 hours and up to 10 days. (8) Corrosion tests on Inconel 693 and K-3 refractory at temperatures between 1000 and 1050 deg. C indicate that both materials should be suitable for melting iron phosphate glasses. (9) The viscosity and electrical conductivity of the MS26AZ102F-2 melt are within the acceptable limits for RSM and CCIM processing. (10)This work has shown that iron phosphate compositions are a potential alternative to borosilicate glasses for vitrifying problematic wastes such as Hanford AZ-102 LAW that contains high amounts sulfate and alkali oxides, and that iron phosphate melts such as MS26AZ102F-2 can be processed in the JHM or CCIM. (authors)},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {7}
}

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