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Title: DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS

Abstract

Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium aqueous radioactive wastes. The addition of clay and a catalyst as co-reactants converts high sodium aqueous low activity wastes (LAW) such as those existing at the Hanford and Idaho DOE sites to a granular ''mineralized'' waste form that may be made into a monolith form if necessary. Simulant Hanford and Idaho high sodium wastes were processed in a pilot scale FBSR at Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low-activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium-bearing waste (SBW). The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The durability of the FBSR waste form products was tested in order to compare the measured durability to previous FBSR waste form testing on Hanford Envelope C waste forms that were made by THOR Treatment Technologiesmore » (TTT) and to compare the FBSR durability to vitreous LAW waste forms, specifically the Hanford low activity waste (LAW) glass known as the Low-activity Reference Material (LRM). The durability of the FBSR waste form is comparable to that of the LRM glass for the test responses studied.« less

Authors:
Publication Date:
Research Org.:
SRS
Sponsoring Org.:
USDOE
OSTI Identifier:
890052
Report Number(s):
WSRC-MS-2006-00015
TRN: US0604696
DOE Contract Number:
DE-AC09-96SR18500
Resource Type:
Conference
Resource Relation:
Conference: Not Available
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; CATALYSTS; CLAYS; FLUIDIZED BEDS; GLASS; LEACHING; MINERAL WASTES; RADIOACTIVE WASTES; SODIUM; STEAM; TESTING; US EPA; WASTE FORMS; WASTE MANAGEMENT; WASTES

Citation Formats

Jantzen, C. DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS. United States: N. p., 2006. Web.
Jantzen, C. DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS. United States.
Jantzen, C. Fri . "DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS". United States. doi:. https://www.osti.gov/servlets/purl/890052.
@article{osti_890052,
title = {DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS},
author = {Jantzen, C},
abstractNote = {Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium aqueous radioactive wastes. The addition of clay and a catalyst as co-reactants converts high sodium aqueous low activity wastes (LAW) such as those existing at the Hanford and Idaho DOE sites to a granular ''mineralized'' waste form that may be made into a monolith form if necessary. Simulant Hanford and Idaho high sodium wastes were processed in a pilot scale FBSR at Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low-activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium-bearing waste (SBW). The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The durability of the FBSR waste form products was tested in order to compare the measured durability to previous FBSR waste form testing on Hanford Envelope C waste forms that were made by THOR Treatment Technologies (TTT) and to compare the FBSR durability to vitreous LAW waste forms, specifically the Hanford low activity waste (LAW) glass known as the Low-activity Reference Material (LRM). The durability of the FBSR waste form is comparable to that of the LRM glass for the test responses studied.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Jan 06 00:00:00 EST 2006},
month = {Fri Jan 06 00:00:00 EST 2006}
}

Conference:
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  • Fluidized Bed Steam Reforming (FBSR) is being considered as a mineralizing technology for the immobilization of a wide variety of wastes that are high in organics, nitrates-nitrites, halides, and/or sulfates. These wastes include the decontaminated High Level Waste (HLW) supernates referred to as low activity waste (LAW) at Department of Energy (DOE) sites in the United States and waste streams that may be generated by the advanced nuclear fuel cycle flowsheets that are being considered by the Global Nuclear Energy Partnership (GNEP) initiative. The organics are pyrolyzed into CO{sub 2} and steam in the absence of air. The FBSR mineralmore » waste form is a granular but can subsequently be made into a monolith for disposal if necessary. The waste form is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals (sodalite, nosean, and nepheline) with cage and ring structures that sequester radionuclides like Tc-99 and Cs-137 and anions such as SO{sub 4}, I, F, and Cl. Iron bearing spinel minerals are also formed and these phases stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Dissolution rates ({eta}) and activation energies of dissolution are parameters needed for Performance Assessments (PA) to be completed on the FBSR mineral waste form. These parameters are defined in this study by Single Pass Flow Through (SPFT) testing. The dissolution rate ({eta}) and the activation energies for dissolution calculated in this study agree with the available rate and activation energy data for natural single crystal nepheline. (authors)« less
  • The Savannah River National Laboratory (SRNL) was requested to generate a document for the Washington State Department of Ecology and the U.S. Environmental Protection Agency that would cover the following topics: (1) A description of the mineral structures produced by Fluidized Bed Steam Reforming (FBSR) of Hanford type Low Activity Waste (LAW including LAWR which is LAW melter recycle waste) waste, especially the cage structured minerals and how they are formed. (2) How the cage structured minerals contain some contaminants, while others become part of the mineral structure (Note that all contaminants become part of the mineral structure and thismore » will be described in the subsequent sections of this report). (3) Possible contaminant release mechanisms from the mineral structures. (4) Appropriate analyses to evaluate these release mechanisms. (5) Why the appropriate analyses are comparable to the existing Hanford glass dataset. In order to discuss the mineral structures and how they bond contaminants a brief description of the structures of both mineral (ceramic) and vitreous waste forms will be given to show their similarities. By demonstrating the similarities of mineral and vitreous waste forms on atomic level, the contaminant release mechanisms of the crystalline (mineral) and amorphous (glass) waste forms can be compared. This will then logically lead to the discussion of why many of the analyses used to evaluate vitreous waste forms and glass-ceramics (also known as glass composite materials) are appropriate for determining the release mechanisms of LAW/LAWR mineral waste forms and how the durability data on LAW/LAWR mineral waste forms relate to the durability data for LAW/LAWR glasses. The text will discuss the LAW mineral waste form made by FBSR. The nanoscale mechanism by which the minerals form will be also be described in the text. The appropriate analyses to evaluate contaminant release mechanisms will be discussed, as will the FBSR test results to date and how they compare to testing performed on LAW glasses. Other details about vitreous waste form durability and impacts of REDuction/OXidation (REDOX) on durability are given in Appendix A. Details about the FBSR process, various pilot scale demonstrations, and applications are given in Appendix B. Details describing all the different leach tests that need to be used jointly to determine the leaching mechanisms of a waste form are given in Appendix C. Cautions regarding the way in which the waste form surface area is measured and in the choice of leachant buffers (if used) are given in Appendix D.« less
  • Fluidized Bed Steam Reforming (FBSR) processing of Sodium Bearing Waste simulants was performed in December 2006 by THOR{sup sm} Treatment Technologies LLC (TTT) The testing was performed at the Hazen Research Inc. (HRI) pilot plant facilities in Golden, CO. FBSR products from these pilot tests on simulated waste representative of the SBW at the Idaho Nuclear Technology and Engineering Center (INTEC) were subsequently transferred to the Savannah River National Laboratory (SRNL) for characterization and leach testing. Four as-received Denitration and Mineralization Reformer (DMR) granular/powder samples and four High Temperature Filter (HTF) powder samples were received by SRNL. FBSR DMR samplesmore » had been taken from the ''active'' bed, while the HTF samples were the fines collected as carryover from the DMR. The process operated at high fluidizing velocities during the mineralization test such that nearly all of the product collected was from the HTF. Active bed samples were collected from the DMR to monitor bed particle size distribution. Characterization of these crystalline powder samples shows that they are primarily Al, Na and Si, with > 1 wt% Ca, Fe and K. The DMR samples contained less than 1 wt% carbon and the HTF samples ranged from 13 to 26 wt% carbon. X-ray diffraction analyses show that the DMR samples contained significant quantities of the Al{sub 2}O{sub 3} startup bed. The DMR samples became progressively lower in starting bed alumina with major Na/Al/Si crystalline phases (nepheline and sodium aluminosilicate) present as cumulative bed turnover occurred but 100% bed turnover was not achieved. The HTF samples also contained these major crystalline phases. Durability testing of the DMR and HTF samples using the ASTM C1285 Product Consistency Test (PCT) 7-day leach test at 90 C was performed along with several reference glass samples. Comparison of the normalized leach rates for the various DMR and HTF components was made with the reference glasses and the Low Activity Waste (LAW) specification for the Hanford Waste Treatment and Vitrification Plant (WTP). Normalized releases from the DMR and HTF samples were all less than 1 g/m{sup 2}. For comparison, normalized release from the High-Level Waste (HLW) benchmark Environmental Assessment (EA) glass for Si, Li, Na and B ranges from 2 to 8 g/m{sup 2}. The normalized release specification for LAW glass for the Hanford WTP is 2 g/m{sup 2}. The Toxicity Characteristic Leach Test (TCLP) was performed on DMR and HTF as received samples and the tests showed that these products meet the criteria for the EPA RCRA Universal Treatment Standards for all of the constituents contained in the starting simulants such as Cr, Pb and Hg (RCRA characteristically hazardous metals) and Ni and Zn (RCRA metals required for listed wastes).« less
  • The U.S. Department of Energy’s Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford’s tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in themore » time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. In addition, the WTP LAW vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as 137Cs, 129I, 99Tc, Cl, F, and SO4 that volatilize at the vitrification temperature of 1150°C in the absence of a continuous cold cap (that could minimize volatilization). The current waste disposal path for the WTP-SW is to process it through the Effluent Treatment Facility (ETF). Fluidized Bed Steam Reforming (FBSR) is being considered for immobilization of the ETF concentrate that would be generated by processing the WTP-SW. The focus of this current report is the WTP-SW.« less
  • Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium low activity wastes (LAW) such as those existing at the Hanford site, at the Idaho National Laboratory (INL), and the Savannah River Site (SRS). The addition of clay, charcoal, and a catalyst as co-reactants with the waste denitrates the aqueous wastes and forms a granular mineral waste form that can subsequently be made into a monolith for disposal if necessary. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage and ringmore » structures and iron bearing spinel minerals. The mineralization occurs at moderate temperatures between 650-750 C in the presence of superheated steam. The cage and ring structured feldspathoid minerals atomically bond radionuclides like Tc-99 and Cs-137 and anions such as SO{sub 4}, I, F, and Cl. The spinel minerals stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium bearing waste (SBW) in pilot scale facilities at the Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The results of the SPFT testing and the activation energies for dissolution are discussed in this study.« less