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Title: Mercury Phase II Study - Mercury Behavior in Salt Processing Flowsheet

Abstract

Mercury (Hg) in the Savannah River Site Liquid Waste System (LWS) originated from decades of canyon processing where it was used as a catalyst for dissolving the aluminum cladding of reactor fuel. Approximately 60 metric tons of mercury is currently present throughout the LWS. Mercury has long been a consideration in the LWS, from both hazard and processing perspectives. In February 2015, a Mercury Program Team was established at the request of the Department of Energy to develop a comprehensive action plan for long-term management and removal of mercury. Evaluation was focused in two Phases. Phase I activities assessed the Liquid Waste inventory and chemical processing behavior using a system-by-system review methodology, and determined the speciation of the different mercury forms (Hg+, Hg++, elemental Hg, organomercury, and soluble versus insoluble mercury) within the LWS. Phase II activities are building on the Phase I activities, and results of the LWS flowsheet evaluations will be summarized in three reports: Mercury Behavior in the Salt Processing Flowsheet (i.e. this report); Mercury Behavior in the Defense Waste Processing Facility (DWPF) Flowsheet; and Mercury behavior in the Tank Farm Flowsheet (Evaporator Operations). The evaluation of the mercury behavior in the salt processing flowsheet indicates, intermore » alia, the following: (1) In the assembled Salt Batches 7, 8 and 9 in Tank 21, the total mercury is mostly soluble with methylmercury (MHg) contributing over 50% of the total mercury. Based on the analyses of samples from 2H Evaporator feed and drop tanks (Tanks 38/43), the source of MHg in Salt Batches 7, 8 and 9 can be attributed to the 2H evaporator concentrate used in assembling the salt batches. The 2H Evaporator is used to evaporate DWPF recycle water. (2) Comparison of data between Tank 21/49, Salt Solution Feed Tank (SSFT), Decontaminated Salt Solution Hold Tank (DSSHT), and Tank 50 samples suggests that the total mercury as well as speciated forms in the assembled salt batches in Tanks 21/49 pass through the Actinide Removal Process (ARP) / Modular Caustic Side Solvent Extraction Unit (MCU) process to Tank 50 with no significant change in the mercury chemistry. (3) In Tank 50, Decontaminated Salt Solution (DSS) from ARP/MCU is the major contributor to the total mercury including MHg. (4) Speciation analyses of TCLP leached solutions of the grout samples prepared from Tank 21, as well as Tank 50 samples, show the majority of the mercury released in the solution is MHg.« less

Authors:
 [1];  [2];  [3];  [3]
  1. Savannah River Remediation, LLC., Aiken, SC (United States)
  2. Savannah River Remediation, LLC., Aiken, SC (United States). Sludge and Salt Planning
  3. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Remediation, LLC., Aiken, SC (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1281779
Report Number(s):
SRR-CES-2016-00005
TRN: US1601671
DOE Contract Number:
AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; MERCURY; FLOWSHEETS; TANKS; SOLUTIONS; SALTS; LIQUID WASTES; SAVANNAH RIVER PLANT; SOLVENT EXTRACTION; EVAPORATORS; METHYLMERCURY; REMOVAL; CHEMICAL PROPERTIES; RADIOACTIVE WASTE PROCESSING

Citation Formats

Jain, V., Shah, H., Bannochie, C. J., and Wilmarth, W. R. Mercury Phase II Study - Mercury Behavior in Salt Processing Flowsheet. United States: N. p., 2016. Web. doi:10.2172/1281779.
Jain, V., Shah, H., Bannochie, C. J., & Wilmarth, W. R. Mercury Phase II Study - Mercury Behavior in Salt Processing Flowsheet. United States. doi:10.2172/1281779.
Jain, V., Shah, H., Bannochie, C. J., and Wilmarth, W. R. 2016. "Mercury Phase II Study - Mercury Behavior in Salt Processing Flowsheet". United States. doi:10.2172/1281779. https://www.osti.gov/servlets/purl/1281779.
@article{osti_1281779,
title = {Mercury Phase II Study - Mercury Behavior in Salt Processing Flowsheet},
author = {Jain, V. and Shah, H. and Bannochie, C. J. and Wilmarth, W. R.},
abstractNote = {Mercury (Hg) in the Savannah River Site Liquid Waste System (LWS) originated from decades of canyon processing where it was used as a catalyst for dissolving the aluminum cladding of reactor fuel. Approximately 60 metric tons of mercury is currently present throughout the LWS. Mercury has long been a consideration in the LWS, from both hazard and processing perspectives. In February 2015, a Mercury Program Team was established at the request of the Department of Energy to develop a comprehensive action plan for long-term management and removal of mercury. Evaluation was focused in two Phases. Phase I activities assessed the Liquid Waste inventory and chemical processing behavior using a system-by-system review methodology, and determined the speciation of the different mercury forms (Hg+, Hg++, elemental Hg, organomercury, and soluble versus insoluble mercury) within the LWS. Phase II activities are building on the Phase I activities, and results of the LWS flowsheet evaluations will be summarized in three reports: Mercury Behavior in the Salt Processing Flowsheet (i.e. this report); Mercury Behavior in the Defense Waste Processing Facility (DWPF) Flowsheet; and Mercury behavior in the Tank Farm Flowsheet (Evaporator Operations). The evaluation of the mercury behavior in the salt processing flowsheet indicates, inter alia, the following: (1) In the assembled Salt Batches 7, 8 and 9 in Tank 21, the total mercury is mostly soluble with methylmercury (MHg) contributing over 50% of the total mercury. Based on the analyses of samples from 2H Evaporator feed and drop tanks (Tanks 38/43), the source of MHg in Salt Batches 7, 8 and 9 can be attributed to the 2H evaporator concentrate used in assembling the salt batches. The 2H Evaporator is used to evaporate DWPF recycle water. (2) Comparison of data between Tank 21/49, Salt Solution Feed Tank (SSFT), Decontaminated Salt Solution Hold Tank (DSSHT), and Tank 50 samples suggests that the total mercury as well as speciated forms in the assembled salt batches in Tanks 21/49 pass through the Actinide Removal Process (ARP) / Modular Caustic Side Solvent Extraction Unit (MCU) process to Tank 50 with no significant change in the mercury chemistry. (3) In Tank 50, Decontaminated Salt Solution (DSS) from ARP/MCU is the major contributor to the total mercury including MHg. (4) Speciation analyses of TCLP leached solutions of the grout samples prepared from Tank 21, as well as Tank 50 samples, show the majority of the mercury released in the solution is MHg.},
doi = {10.2172/1281779},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2016,
month = 7
}

Technical Report:

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  • An evaluation of the previous Chemical Processing Cell (CPC) testing was performed to determine whether the planned concurrent operation, or “coupled” operations, of the Defense Waste Processing Facility (DWPF) with the Salt Waste Processing Facility (SWPF) has been adequately covered. Tests with the nitricglycolic acid flowsheet, which were both coupled and uncoupled with salt waste streams, included several tests that required extended boiling times. This report provides the evaluation of previous testing and the testing recommendation requested by Savannah River Remediation. The focus of the evaluation was impact on flammability in CPC vessels (i.e., hydrogen generation rate, SWPF solvent components,more » antifoam degradation products) and processing impacts (i.e., acid window, melter feed target, rheological properties, antifoam requirements, and chemical composition).« less
  • The Mercury Program team’s effort continues to develop more fundamental information concerning mercury behavior across the liquid waste facilities and unit operations. Previously, the team examined the mercury chemistry across salt processing, including the Actinide Removal Process/Modular Caustic Side Solvent Extraction Unit (ARP/MCU), and the Defense Waste Processing Facility (DWPF) flowsheets. This report documents the data and understanding of mercury across the high level waste 2H and 3H evaporator systems.
  • The purpose of this report is to provide a summary of the DWPF processing history in regards to mercury, document the mercury results obtained on the product and condensate samples, and provide further recommendations based on the data obtained.
  • A tentative flowsheet for fused fluoride salt dissolution of U - Zr fuel material is presented. (T.R.H)
  • The High Level Waste (HLW) Salt Disposition Systems Engineering Team was formed on March 13, 1998, and chartered to identify options, evaluate alternatives, and recommend a selected alternative(s) for processing HLW salt to a permitted wasteform. This requirement arises because the existing In-Tank Precipitation process at the Savannah River Site, as currently configured, cannot simultaneously meet the HLW production and Authorization Basis safety requirements. This engineering study was performed in four phases. This document provides the technical bases, assumptions, and results of this engineering study.