RADIOACTIVE DEMONSTRATION OF FINAL MINERALIZED WASTE FORMS FOR HANFORD WASTE TREATMENT PLANT SECONDARY WASTE BY FLUIDIZED BED STEAM REFORMING USING THE BENCH SCALE REFORMER PLATFORM

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 the 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 {sup 137}Cs, {sup 129}I, {sup 99}Tc, Cl, F, and SO{sub 4} 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. FBSR offers a moderate temperature (700-750 C) continuous method by which WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline ceramic (mineral) waste form. The mineral waste form that is produced by co-processing waste with kaolin clay in an FBSR process has been shown to be as durable as LAW glass. Monolithing of the granular FBSR product is being investigated to prevent dispersion during transport or burial/storage, but is not necessary for performance. A Benchscale Steam Reformer (BSR) was designed and constructed at the SRNL to treat actual radioactive wastes to confirm the findings of the non-radioactive FBSR pilot scale tests and to qualify the waste form for applications at Hanford. BSR testing with WTP SW waste surrogates and associated analytical analyses and tests of granular products (GP) and monoliths began in the Fall of 2009, and then was continued from the Fall of 2010 through the Spring of 2011. Radioactive testing commenced in 2010 with a demonstration of Hanford's WTP-SW where Savannah River Site (SRS) High Level Waste (HLW) secondary waste from the Defense Waste Processing Facility (DWPF) was shimmed with a mixture of {sup 125/129}I and {sup 99}Tc to chemically resemble WTP-SW. Prior to these radioactive feed tests, non-radioactive simulants were also processed. Ninety six grams of radioactive granular product were made for testing and comparison to the non-radioactive pilot scale tests. The same mineral phases were found in the radioactive and non-radioactive testing.

[1]  Arlin Olson Report for Treating Hanford LAW and WTP SW Simulants: Pilot Plant Mineralizing Flowsheet , 2012 .

[2]  K. M. Goff,et al.  Characterization of a Ceramic Waste Form Encapsulating Radioactive Electrorefiner Salt , 1999 .

[3]  C Jantzen FLUIDIZED BED STEAM REFORMER MONOLITH FORMATION , 2006 .

[4]  Carol M. Jantzen,et al.  Engineering Study of the Hanford Low Activity Waste (LAW) Steam Reforming Process , 2002 .

[5]  Arlin L. Olson,et al.  Fluidized Bed Steam Reforming of Hanford LAW Using THORsm Mineralizing Technology , 2004 .

[6]  F. M. Mann Risk Assessment supporting the decision on the initial selection of supplemental ILAW technologies , 2003 .

[7]  Shas V. Mattigod,et al.  Synthesis and Structure of Perrhenate Sodalite , 2006 .

[8]  C. M. Jantzen,et al.  Characterization and Performance of Fluidized Bed Steam Reforming (FBSR) Product as a Final Waste Form , 2003 .

[9]  C. A. Nash,et al.  Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank Farm Blend) By Fluidized Bed Steam Reformation (FBSR) , 2013 .

[10]  Stephen G. Johnson,et al.  Characterization of a glass-bonded ceramic waste form loaded with U and Pu , 1999 .

[11]  William L. Ebert,et al.  An interlaboratory study of a standard glass for acceptance testing of low-activity waste glass , 2000 .

[12]  Carol M. Jantzen,et al.  Durability Testing of Fluidized Bed Steam Reforming (FBSR) Products , 2012 .

[13]  John Crank,et al.  The Mathematics Of Diffusion , 1956 .

[14]  R. Howie,et al.  Rock-forming minerals , 1962 .

[15]  Edward Salisbury Dana,et al.  A Textbook of Mineralogy , 1991 .

[16]  Carol M. Jantzen,et al.  DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS , 2006 .

[17]  Nikolla P. Qafoku,et al.  Secondary Waste Form Down-Selection Data Package—Fluidized Bed Steam Reforming Waste Form , 2011 .

[18]  C. M. Jantzen,et al.  MINERALIZATION OF RADIOACTIVE WASTES BY FLUIDIZED BED STEAM REFORMING (FBSR): COMPARISONS TO VITREOUS WASTE FORMS, AND PERTINENT DURABILITY TESTING , 2008 .

[19]  W. S. Ginell,et al.  ULTIMATE DISPOSAL OF RADIOACTIVE WASTES , 1954 .

[20]  Carolm. Jantzen,et al.  Disposition of Tank 48H Organics by Fluidized Bed Steam Reforming (FBSR) , 2003 .

[21]  Carol M. Jantzen,et al.  Fluidized Bed Steam Reformed (FBSR) Mineral Waste Forms: Characterization and Durability Testing , 2006 .

[22]  Rodney C. Ewing,et al.  Radioactive Waste Forms for the Future , 1988 .

[23]  J. M. Pareizs,et al.  Single-Pass Flow Through (SPFT) Testing of Fluidized-Bed Steam Reforming (FBSR) Waste Forms , 2005 .

[24]  Carol M. Jantzen,et al.  FLUIDIZED BED STEAM REFORMER (FBSR) PRODUCT: MONOLITH FORMATION AND CHARACTERIZATION , 2006 .

[25]  P Burket STEAM REFORMING TECHNOLOGY DEMONSTRATION FOR THE DESTRUCTION OF ORGANICS ON ACTUAL DOE SAVANNAH RIVER SITE TANK 48H WASTE 9138 , 2009 .

[26]  C. L. Crawford,et al.  Evaluation of THOR™Mineralized Waste Forms (Granular and Monolith) for the DOE Advanced Remediation Technologies (ART) Phase 2 Project , 2010 .

[27]  R. M. Barrer,et al.  Hydrothermal Chemistry of Zeolites , 1982 .

[28]  S. Brantley,et al.  Surface area and porosity of primary silicate minerals , 2000 .