[en] This document completes the requirements of Milestone 1-2, PNNL Draft Literature Review, discussed in the scope of work outlined in the EM-31 Support Project task plan WP-2.3.6-2010-1. The focus of task WP 2.3.6 is to improve the U.S. Department of Energy's (DOE's) understanding of filtration operations for high-level waste (HLW) to enhance filtration and cleaning efficiencies, thereby increasing process throughput and reducing the sodium demand (through acid neutralization). Developing the processes for fulfilling the cleaning/backpulsing requirements will result in more efficient operations for both the Hanford Tank Waste Treatment and Immobilization Plant (WTP) and the Savannah River Site (SRS), thereby increasing throughput by limiting cleaning cycles. The purpose of this document is to summarize Pacific Northwest National Laboratory's (PNNL's) literature review of historical filtration testing at the laboratory and of testing found in peer-reviewed journals. Eventually, the contents of this document will be merged with a literature review by SRS to produce a summary report for DOE of the results of previous filtration testing at the laboratories and the types of testing that still need to be completed to address the questions about improved filtration performance at WTP and SRS. To this end, this report presents (1) a review of the current state of crossflow filtration knowledge available in the peer-reviewed literature, (2) a detailed review of PNNL-related filtration studies specific to the Hanford site, and (3) an overview of current waste filtration models developed by PNNL and suggested avenues for future model development.

[en] A series of leach tests were performed on actual Hanford Site tank wastes in support of the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The samples were targeted composite slurries of high-level tank waste materials representing major complex, radioactive, tank waste mixtures at the Hanford Site. Using a filtration/leaching apparatus, sample solids were concentrated, caustic leached, and washed under conditions representative of those planned for the Pretreatment Facility in the WTP. Caustic leaching was performed to assess the mobilization of aluminum (as gibbsite, Al(OH)3, and boehmite AlO(OH)), phosphates (PO43-), chromium (Cr3+) and, to a lesser extent, oxalates (C2O42-). Ferrocyanide waste released the solid phase 137Cs during caustic leaching; this was antithetical to the other Hanford waste types studied. Previous testing on ferrocyanide tank waste focused on the aging of the ferrocyanide salt complex and its thermal compatibilities with nitrites and nitrates. Few studies, however, examined cesium mobilization in the waste. Careful consideration should be given to the pretreatment of ferrocyanide wastes in light of this new observed behavior, given the fact that previous testing on simulants indicates a vastly different cesium mobility in this waste form. The discourse of this work will address the overall ferrocyanide leaching characteristics as well as the behavior of the 137Cs during leaching.

[en] The Waste Treatment Plant currently under construction for treatment of High Level Waste at the Hanford Site will process High Level Waste (HLW) to reduce the quantity of HLW material that must be immobilized. Recently, an extensive testing program was undertaken to characterize the composition of some of the major sources of HLW in the Hanford tank farm system. This effort has led to an increased understanding of the chemical form and the underlying dissolution chemistry for much of the waste.

[en] Crossflow filtration is to be a key process in the treatment and disposal of approximately 60,000 metric tons of high-level radioactive waste stored at the Hanford Site in Richland, Washington. Pacific Northwest National Laboratory is assessing filter performance with waste simulant materials that mimic the chemical and physical properties of Hanford tank waste. Prior simulant studies indicated that waste filtration performance may be limited by pore and cake fouling. To limit the shutdown of waste treatment operations, the pre-treatment facility plans to recover filter flux losses from cake formation and filter fouling by frequently backpulsing the filter elements. The objective of the current paper is to develop a simple model of flux decline resulting from cake and pore fouling and potential flux recovery through backpulsing of the filters for Hanford waste filtration operations. To this end, a model capable of characterizing the decline in waste-simulant filter flux as a function of both irreversible pore blockage and reversible cake formation is proposed. This model is used to characterize the filtration behavior of Hanford waste simulants in both continuous and backpulsed operations. The model is then used to infer the optimal backpulse frequency under specific operating conditions.

[en] The Waste Treatment and Immobilization Plant (WTP) currently under construction for treatment of High-Level Waste (HLW) at the Hanford Site will rely on cross-flow ultrafiltration to provide solids-liquid separation as a core part of the treatment process. To optimize process throughput, periodic chemical cleaning of the porous stainless steel filter elements has been incorporated into the design of the plant. It is currently specified that chemical cleaning with nitric acid will occur after significant irreversible membrane fouling is observed. Irreversible fouling is defined as fouling that cannot be removed by backpulsing the filter. PNNL has investigated chemical cleaning processes as part of integrated tests with HLW simulants and with actual Hanford tank wastes. To quantify the effectiveness of chemical cleaning, the residual membrane resistance after cleaning was compared against the initial membrane resistance for each test in a series of long-term fouling tests. The impact of the small amount of residual resistance in these tests could not be separated from other parameters and the historical benchmark of >1 GPM/ft2 for clean water flux was determined to be an adequate metric for chemical cleaning. Using the results from these tests, a process optimization strategy is presented suggesting that for the simulant material under test, the value of chemical cleaning may be suspect. The period of enhanced filtration may not be enough to offset the down time required for chemical cleaning, without respect to the other associated costs.

[en] This is the final report in a series of eight reports defining characterization, leach, and filtration testing of a wide variety of Hanford tank waste sludges. The information generated from this series is intended to supplement the Waste Treatment and Immobilization Plant (WTP) project understanding of actual waste behaviors associated with tank waste sludge processing through the pretreatment portion of the WTP. The work described in this report presents information on a high-iron waste form, specifically the ferrocyanide tank waste sludge. Iron hydroxide has been shown to pose technical challenges during filtration processing; the ferrocyanide tank waste sludge represented a good source of the high-iron matrix to test the filtration processing

[en] This report describes the bench-scale pretreatment processing of actual tank waste materials through the entire baseline WTP pretreatment flowsheet in an effort to demonstrate the efficacy of the defined leaching processes on actual Hanford tank waste sludge and the potential impacts on downstream pretreatment processing. The test material was a combination of reduction oxidation (REDOX) tank waste composited materials containing aluminum primarily in the form of boehmite and dissolved S saltcake containing Cr(III)-rich entrained solids. The pretreatment processing steps tested included: caustic leaching for Al removal; solids crossflow filtration through the cell unit filter (CUF); stepwise solids washing using decreasing concentrations of sodium hydroxide with filtration through the CUF; oxidative leaching using sodium permanganate for removing Cr; solids filtration with the CUF; follow-on solids washing and filtration through the CUF; ion exchange processing for Cs removal; evaporation processing of waste stream recycle for volume reduction; and combination of the evaporated product with dissolved saltcake. The effectiveness of each process step was evaluated by following the mass balance of key components (such as Al, B, Cd, Cr, Pu, Ni, Mn, and Fe), demonstrating component (Al, Cr, Cs) removal, demonstrating filterability by evaluating filter flux rates under various processing conditions (transmembrane pressure, crossflow velocities, wt% undissolved solids, and PSD) and filter fouling, and identifying potential issues for WTP. The filterability was reported separately (Shimskey et al. 2008) and is not repeated herein

[en] A testing program evaluating actual tank waste was developed in response to Task 4 from the M-12 External Flowsheet Review Team (EFRT) issue response plan.() The test program was subdivided into logical increments. The bulk water-insoluble solid wastes that are anticipated to be delivered to the Waste Treatment and Immobilization Plant (WTP) were identified according to type such that the actual waste testing could be targeted to the relevant categories. Eight broad waste groupings were defined. Samples available from the 222S archive were identified and obtained for testing. The actual waste-testing program included homogenizing the samples by group, characterizing the solids and aqueous phases, and performing parametric leaching tests. Two of the eight defined groups - bismuth phosphate sludge (Group 1) and bismuth phosphate saltcake (Group 2) - are the subjects of this report. The Group 1 waste was anticipated to be high in phosphorus and was implicitly assumed to be present as BiPO4 (however, results presented here indicate that the phosphate in Group 1 is actually present as amorphous iron(III) phosphate). The Group 2 waste was also anticipated to be high in phosphorus, but because of the relatively low bismuth content and higher aluminum content, it was anticipated that the Group 2 waste would contain a mixture of gibbsite, sodium phosphate, and aluminum phosphate. Thus, the focus of the Group 1 testing was on determining the behavior of P removal during caustic leaching, and the focus of the Group 2 testing was on the removal of both P and Al. The waste-type definition, archived sample conditions, homogenization activities, characterization (physical, chemical, radioisotope, and crystal habit), and caustic leaching behavior as functions of time, temperature, and hydroxide concentration are discussed in this report. Testing was conducted according to TP-RPP-WTP-467

[en] A testing program evaluating actual tank waste was developed in response to Task 4 from the M-12 External Flowsheet Review Team (EFRT) issue response plan. The test program was subdivided into logical increments. The bulk water-insoluble solid wastes that are anticipated to be delivered to the Waste Treatment and Immobilization Plant (WTP) were identified according to type such that the actual waste testing could be targeted to the relevant categories. Under test plan TP-RPP-WTP-467, eight broad waste groupings were defined. Samples available from the 222S archive were identified and obtained for testing. Under this test plan, a waste-testing program was implemented that included: (sm_bullet) Homogenizing the archive samples by group as defined in the test plan (sm_bullet) Characterizing the homogenized sample groups (sm_bullet) Performing parametric leaching testing on each group for compounds of interest (sm_bullet) Performing bench-top filtration/leaching tests in the hot cell for each group to simulate filtration and leaching activities if they occurred in the UFP2 vessel of the WTP Pretreatment Facility. This report focuses on filtration/leaching tests performed on two of the eight waste composite samples and follow-on parametric tests to support aluminum leaching results from those tests.

[en] Fluor Hanford is responsible for cleanup of legacy wastes, old production facilities, and environmental contamination that remain at the Hanford site. New technologies and technical information are being introduced to improve cost efficiency and assure safety. This paper presents recent advances in four of Fluor's projects. Supporting the Plutonium Finishing Plan Closure Project, laboratory evaluations and thermal analyses were conducted to quantify the potential for self-heating reactions that can develop in materials used to remove plutonium from contaminated equipment. Four commercial products were tested, and safe limits for packaging these wastes have been developed. The Groundwater Remediation Project is testing two technologies that show promise of preventing groundwater contaminants from reaching the Columbia River by innovative in situ methods. Laboratory tests are showing that the mineral apatite can sequester Sr-90, and current work to control in situ placement of the barrier is supporting a field deployment in late FY 06. In another location, a new approach using zero valent iron is being tested to 'mend' areas breached in the in situ redox manipulation barrier, which was installed to convert soluble chromium +6 to the less mobile +3 state. The Waste Stabilization and Disposition Project has successfully operated a process to grout sludge from spent fuel storage basins which controls the dose below contact handled limits. An in-line sensor and a nomogram that correlates dose to curies provide the operators with a simple and effective method to assure all waste drums meet WIPP acceptance specifications. The K Basins Closure Project will be transferring sludge containing fuel fragments using hoses and several pump booster stations. Selection of equipment fabrication materials required testing with a simulant, which in turn required laboratory evaluations of irradiated fuel hardness so that an appropriate non-radioactive material could be selected. A tungsten alloy was selected and used for testing system components