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Title: FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING

Abstract

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 ring 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 SO4, 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 Applicationsmore » 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

Authors:
; ; ;
Publication Date:
Research Org.:
SRS
Sponsoring Org.:
USDOE
OSTI Identifier:
902181
Report Number(s):
WSRC-STI-2006-00317
TRN: US0702804
DOE Contract Number:
DE-AC09-96SR18500
Resource Type:
Conference
Resource Relation:
Conference: Scientific Basis for Nuclear Waste Managment XXX
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; ANIONS; BEARINGS; CATALYSTS; CHARCOAL; DISSOLUTION; FLUIDIZED BEDS; IRON; LEACHING; MINERAL WASTES; MINERALIZATION; RADIOACTIVE WASTES; RADIOISOTOPES; RESOURCE CONSERVATION; SODIUM; SPINELS; STEAM; TESTING; US EPA; WASTE FORMS

Citation Formats

Jantzen, C, Troy Lorier, T, John Pareizs, J, and James Marra, J. FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING. United States: N. p., 2007. Web.
Jantzen, C, Troy Lorier, T, John Pareizs, J, & James Marra, J. FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING. United States.
Jantzen, C, Troy Lorier, T, John Pareizs, J, and James Marra, J. Sat . "FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING". United States. doi:. https://www.osti.gov/servlets/purl/902181.
@article{osti_902181,
title = {FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING},
author = {Jantzen, C and Troy Lorier, T and John Pareizs, J and James Marra, J},
abstractNote = {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 ring 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 SO4, 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.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sat Mar 31 00:00:00 EDT 2007},
month = {Sat Mar 31 00:00:00 EDT 2007}
}

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  • 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
  • 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
  • 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.more » 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.« less
  • This report describes the benchscale testing with simulant and radioactive Hanford Tank Blends, mineral product characterization and testing, and monolith testing and characterization. These projects were funded by DOE EM-31 Technology Development & Deployment (TDD) Program Technical Task Plan WP-5.2.1-2010-001 and are entitled “Fluidized Bed Steam Reformer Low-Level Waste Form Qualification”, Inter-Entity Work Order (IEWO) M0SRV00054 with Washington River Protection Solutions (WRPS) entitled “Fluidized Bed Steam Reforming Treatability Studies Using Savannah River Site (SRS) Low Activity Waste and Hanford Low Activity Waste Tank Samples”, and IEWO M0SRV00080, “Fluidized Bed Steam Reforming Waste Form Qualification Testing Using SRS Low Activity Wastemore » and Hanford Low Activity Waste Tank Samples”. This was a multi-organizational program that included Savannah River National Laboratory (SRNL), THOR® Treatment Technologies (TTT), Pacific Northwest National Laboratory (PNNL), Oak Ridge National Laboratory (ORNL), Office of River Protection (ORP), and Washington River Protection Solutions (WRPS). The SRNL testing of the non-radioactive pilot-scale Fluidized Bed Steam Reformer (FBSR) products made by TTT, subsequent SRNL monolith formulation and testing and studies of these products, and SRNL Waste Treatment Plant Secondary Waste (WTP-SW) radioactive campaign were funded by DOE Advanced Remediation Technologies (ART) Phase 2 Project in connection with a Work-For-Others (WFO) between SRNL and TTT.« 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