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At least 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Enhanced prediction of Cs removal by CST from Hanford tank waste with K accountability

Abstract The treatment of Hanford tank waste is one of the most challenging environmental cleanup activities to date. To expedite the processing of liquid waste stored in underground tanks in Washington State it is necessary to remove the significant dose contributor, 137 Cs. Crystalline silicotitanate ion exchanger is currently used to remove 137 Cs from the aqueous phase of Hanford tank wastes in preparation for vitrification at the Waste Treatment and Immobilization Plant (WTP). Improving the understanding of potassium impacts on ion exchange behavior of Cs will help in the operation of a critical component of one of the most complex treatment processes in the world today. Optimization of this process can result in significant cost savings and less waste production. Toward this effort, a series of batch contact tests varied in potassium concentration were conducted to look at the impact of potassium concentration on Cs distribution. Experimental distribution ratios ( K d ) were compared to the distribution ratios predicted using the ZAM model. A significant underprediction of Cs capacity in the presence of potassium was seen with the existing model. A revision of the equilibrium constants was determined and provided a statistically better fit for determining the Cs K d values in tank waste matrices.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1979

Redox flow cell energy storage systems

NASA-Redox systems are electrochemical storage devices that use two fully soluble Redox couples, anode and cathode fluids, as active electrode materials separated by a highly selective ion exchange membrane. The reactants are contained in large storage tanks and pumped through a stack of Redox flow cells where the electrochemical reactions (reduction and oxidation) take place at porous carbon felt electrodes. A string or stack of these power producing cells is connected in series in a bipolar manner. Redox energy storage systems promise to be inexpensive and possess many features that provide for flexible design, long life, high reliability and minimal operation and maintenance costs. These features include independent sizing of power and storage capacity requirements and inclusion within the cell stack of a cell that monitors the state of charge of the system as a whole, and a rebalance cell which permits continuous correction to be made for minor side reactions that would tend to result in the anode fluid and cathode fluids becoming electrochemically out of balance. These system features are described and discussed.

Thaller, L. H.↗
DOE OSTI2020

Complex magnetic structure in Ba 5 Ru 3 O 12 with isolated Ru 3 O 12 trimer

We report detailed magnetic, transport, heat-capacity, and neutron diffraction measurements of Ba 5 Ru 3 O 12 , a compound consisting of isolated Ru 3 O 12 trimers. We show that this system develops long-range antiferromagnetic ordering at T N ~ 60 K without structural distortion or metal-insulator-type transition, which is in sharp contrast to other Barium Ruthenate trimer systems such as 9R-BaRuO 3 and Ba 4 Ru 3 O 10 . A complex magnetic structure is revealed which is attributable to the magnetic frustration due to competing exchange interactions between Ru ions on different crystallographic sites within the Ru 3 O 12 trimer and different degree of orbital hybridization on different Ru-sites. In conclusion, we have also investigated the magnetic structure of Ba 4 Ru 3 O 10 for comparisons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

FY25 Ion Exchange Processing for the West Area Risk Management (WARM) Project

The West Area Risk Management (WARM) Project was established to enable near-term retrieval and pretreatment of tank waste from Hanford’s 200 West Area and to support deployment of an ion exchange (IX) system capable of producing cesium-depleted supernate suitable for offsite treatment and disposal. The WARM experimental campaign was designed to provide key data for design and operational planning of the 200 W IX system, which plans to utilize crystalline silicotitanate (CST) as the active media for cesium removal. This report documents a comprehensive FY25 experimental campaign designed to produce key technical data required for design and operational planning of the WARM IX system. Testing includes assessing Cs and Sr breakthrough performance in a 4-column system, Cs capacity batch contact testing, phosphate precipitation assessments, reduced-hydroxide feed displacement evaluation, and Sr speciation impacts on Sr removal. The experimental results provide detailed trends in Cs and Sr loading behavior, breakthrough performance across a 4-column staged IX system, distribution profiles within CST beds, and projections of operational flowrates relative to Waste Acceptance Criteria (WAC) limits. Batch contact testing established equilibrium partitioning behavior for the S1–S5 simulants and characterized how matrix chemistry influenced Cs sorption onto CST. Additionally, further evaluations on waste matrix as it pertains to precipitation potential were also determined. Collectively, these datasets support engineering design choices for WARM system throughput and pretreatment planning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Manipulating Cu vacancy in Yb triangular lattice Materials: Investigating the quantum disordered compound CuYbSe 2 and spin glass Cu 2.73 ⁢YbP 2

Yb-based triangular lattice materials have attracted significant attention due to their potential for hosting exotic magnetic quantum states. In this paper, we report the structural, magnetic, and thermodynamic properties of two Yb triangular lattice compounds with vacancy disorder at nonmagnetic Cu sites: CuYbSe 2 and Cu 2.73 ⁢YbP 2 . Single-crystal x-ray diffraction determines notable Cu-site vacancies in both materials. Unlike a single Cu site with 0.5 occupancy in CuYbSe 2 , Cu 2.73 ⁢YbP 2 only presents 27% vacancies on one of three Cu sites. Magnetic susceptibility measurements indicate dominant antiferromagnetic interactions between Yb 3+ ions. The effective magnetic moment is consistent with an effective spin-1/2 state of Yb 3+ . CuYbSe 2 exhibits strong magnetic anisotropy between in-plane and out-of-plane directions with the estimated exchange interactions 𝐽 𝑎 /𝑘 B = 6.48 K and 𝐽 𝑐 /𝑘 B = 2.55 K. No magnetic ordering is observed down to 0.4 K, supporting its quantum disordered ground state and candidacy as a quantum spin liquid. In contrast, Cu 2.73 ⁢YbP 2 shows clear evidence of spin freezing at 4.5 K in both magnetization and heat capacity data, indicating a spin glass state. The field-induced magnetic orders are found in CuYbSe 2 . These results highlight the critical role of structural vacancies in perturbing Yb-based triangular lattices. In conclusion, we demonstrate that while the intrinsic Yb triangular lattices are comparable, the presence of Cu vacancies can fundamentally alter the magnetic ground state—tuning the system between quantum disordered and spin glass behavior.

Frustrated magnetism↗
DOE OSTI2025

Magnetic properties of Tm 3+ in layered triangular lattices

Rare-earth chalcogenides, ARCh 2 (A = alkali metal or monovalent ion; R = rare-earth elements; Ch = O, S, and Se), have been identified as promising candidates for exploring a variety of novel frustrated quantum magnetic phenomena. Tm-based series, ATmCh 2 , where Tm 3+ ions are arranged on various frustrated geometric lattices, provide a platform for investigating the competitions among spin–orbit coupling, crystal field effects, and magnetic exchange interactions in the context of geometric frustration. In this study, we present how the crystallographic structures of newly synthesized ATmSe 2 (A = Li and Na) influence their frustrated magnetic behaviors. Both NaTmSe 2 and LiTmSe 2 adopt a delafossite-type structure with a two-dimensional (2D) triangular lattice, but LiTmSe 2 has a much shorter c-axis parameter compared to this in NaTmSe 2 . Both heat capacity and magnetic susceptibility measurements confirm the absence of long-range magnetic order in either compound. However, magnetic measurements data reveals the differences in magnetic interactions: NaTmSe 2 exhibits features of low-dimensional magnetism, likely driven by its layered crystal structure, compared to LiTmSe 2 .

Crystal field theory↗
DOE OSTI2021

Performance and lifetime of intercalative water deionization cells for mono- and divalent ion removal

We report intercalative deionization (IDI) uses two cation intercalation electrodes separated by an anion exchange membrane in a symmetric cell design that has the potential to deliver electrochemically desalinated water in an energy- and water-efficient way. Here, we define and measure metrics to describe the performance and lifetime of IDI cells and compare them for NaCl and CaCl 2 feed solutions. With 20 mM NaCl, NiHCF/AEM/NiHCF flow cells achieve 10 mM average concentration change at a productivity of 20 l/h/m 2 and 5 mM average concentration change at 130 l/h/m 2 . In both cases the cells are operated at a 3C current rate and consume ~30 Wh/m 3 of energy. With 10 mM CaCl 2 , the specific capacity and salt removal of IDI flow cells is ~4 times lower. NiHCF/NiHCF beaker cells with CaCl 2 electrolyte suffer from strong capacity fade, while the same cells with NaCl electrolyte achieve 500 cycles without any capacity fade. Our post-mortem analysis using X-ray diffraction, secondary electron microscopy, energy dispersive X-ray spectroscopy, synchrotron-based X-ray absorption spectroscopy and micro X-ray fluorescence mapping reveals that NiHCF dissolves upon repeated intercalation with Ca 2+ , releasing residual K + , Ni 2+ and Fe(CN) 6 3 , which precipitates as a crystalline decomposition product on the electrodes. This side reaction deprives the active material NiHCF of charge compensating Fe, and thus accounts for the observed capacity fade.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Characterization of CST Post-Processing AP-105 Hanford Tank Waste

The primary goal of the Tank Side Cesium Removal (TSCR) system, under development by Washington River Protection Solutions, LLC (WRPS), is to remove entrained solids and 137 Cs from the Hanford tank waste supernate to expedite production of low-activity waste. Ion exchange (IX) testing of 10.9 L of waste from Hanford tank 241-AP-105 (AP-105), performed by Pacific Northwest National Laboratory, used a lead-lag-polish column format, with a bed volume of 10 mL per column, to decontaminate tank waste supernate using crystalline silicotitanate (CST) as the IX media. The AP-105 Cs IX processing test, discussed elsewhere, resulted in a shorter transition zone (i.e., steeper load curve) than those defined by wastes from tanks 241-AP-107 and 241-AW-102.1 The shorter transition zone was indicative of a matrix effect retarding Cs capacity. Therefore, aliquots of spent CST from the lead, lag, and polish columns were subjected to a digestion protocol to quantify analytes retained by the CST and extrapolate the impact on Cs capacity. The spent CST was digested using a combination of 5 M HNO 3 and H 2 O 2 with vigorous heating and stirring. Due to the radiation dose accompanying the 137 Cs on the CST columns, a secondary Cs separation by ammonium molybdophosphate embedded in polyacrylonitrile (AMP-PAN) was performed to separate the 137 Cs from the CST so the samples could be contact-handled for analysis outside of a shielded facility.

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NASA NTRS2004

Ionic Liquids and New Proton Exchange Membranes for Fuel Cells

There is currently a great surge of activity in fuel cell research as laboratories across the world seek to take advantage of the high energy capacity provided by &el cells relative to those of other portable electrochemical power systems. Much of this activity is aimed at high temperature fie1 cells, and a vital component of such &el cells must be the availability of a high temperature stable proton-permeable membrane. NASA Glenn Research Center is greatly involved in developing this technology. Other approaches to the high temperature fuel cell involve the use of single- component or almost-single-component electrolytes that provide a path for protons through the cell. A heavily researched case is the phosphoric acid fuel cell, in which the electrolyte is almost pure phosphoric acid and the cathode reaction produces water directly. The phosphoric acid fie1 cell delivers an open circuit voltage of 0.9 V falling to about 0.7 V under operating conditions at 170 C. The proton transport mechanism is mainly vehicular in character according to the viscosity/conductance relation. Here we describe some Proton Transfer Ionic Liquids (PTILs) with low vapor pressure and high temperature stability that have conductivities of unprecedented magnitude for non-aqueous systems. The first requirement of an ionic liquid is that, contrary to experience with most liquids consisting of ions, it must have a melting point that is not much above room temperature. The limit commonly suggested is 100 C. PTILs constitute an interesting class of non-corrosive proton-exchange electrolyte, which can serve well in high temperature (T = 100 - 250 C) fuel cell applications. We will present cell performance data showing that the open circuit voltage output, and the performance of a simple H2(g)Pt/PTIL/Pt/O2(g) fuel cell may be superior to those of the equivalent phosphoric acid electrolyte fuel cell both at ambient temperature and temperatures up to and above 200 C. My work at NASA Glenn Research Center during this summer is to develop and characterize proton exchange membranes doped with ionic liquids. The main techniques used to characterize these materials are: Impedance Spectroscopy, NMR, DSC, TGA, DMA, IR, and SEM ...

Belieres, Jean-Philippe↗
DOE OSTI2021

Uptake of aqueous heavy metal ions (Co2+, Cu2+ and Zn2+) by calcium-aluminium-silicate-hydrate gels

Highlights: • C-A-S-H gels containing metal ions (Co{sup 2+}, Cu{sup 2+} or Zn{sup 2+}) were precipitated by a sol-gel technique. • Uptake mechanism and immobilization capacity of divalent metal ions by C-A-S-H are elucidated. • Up to ~55–60 mol% of Zn can be incorporated in defective tobermorite-type C-A-S-H. • Metal uptake by C-A-S-H is controlled mainly by isomorphous substitution for Ca ions. • Crystal-chemical features of C-A-S-H gels and implications for practical application are discussed. Calcium-aluminium-silicate-hydrate (C-A-S-H) gels containing heavy metal ions (Me: Co{sup 2+}, Cu{sup 2+} or Zn{sup 2+}) were precipitated at different Me/Si molar ratios to study the uptake mechanism and immobilization capacity. Aqueous solution chemistry and solid-phase characterization using XRD, FTIR, ESEM-EDX, TEM-HAADF and TG-DSC methods reveal threshold values for ion substitution of ~55–60 mol% for Zn, ~30–40 mol% for Co and ~25–30 mol% for Cu in defective tobermorite-type C-A-S-H with (Ca + Me)/(Si + Al) molar ratios from 0.86 to 1.04. At higher aqueous Me concentrations, Me (chloride) hydroxides start to co-precipitate. The uptake mechanism of Me ions by C-A-S-H is based on (i) isomorphous substitution of Me for Ca in the CaO layer, (ii) ion exchange in the interlayer, (iii) tetrahedral substitution (Zn) within the dreierketten chains and (iv) surface adsorption onto the C-A-S-H gel structure. Systematics in crystal-chemistry of Me-bearing C-A-S-H and implications for application and performance in natural and man-made settings are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Strong, Yet Split Hydrogen Bonding with Ice Rules in Delafossite (H/D)RhO 2

Despite remaining enigmatic, strong hydrogen bonding provides an advanced design handle for tailoring the properties of functional materials. Here, in this study, 3 R –(H/D)RhO 2 delafossites (prepared by ion exchange of Na + from NaRhO 2 ) contain H/D in linear coordination with O, linking Rh III O 2 layers. Bragg and real-space X-ray and neutron scattering analysis, vibrational and solid-state NMR spectroscopy, and density functional theory (DFT)–based electronic structure calculations have been employed to understand the nature of the hydrogen bonding. Despite short distances between H/D and the two O to which they are bonded, a clear double-minimum corresponding to a shorter and longer (H/D)–O distance is established. The triangular lattices formed by H/D appear to display ice-like disorder, corroborated by low-temperature heat capacity measurements.

NMR spectroscopy↗
DOE OSTI2025

Advancing Pumped Thermal Energy Storage Performance and Cost Using Silica Storage Media

Pumped Thermal Energy Storage (PTES) is an electricity storage system that is suitable for long-duration energy storage (10-1000 h) due to its low marginal cost of energy capacity. We present a techno-economic model of a PTES system that uses particle thermal energy storage. Particles have low costs and can be operated over a wide temperature range leading to increased efficiency and reduced costs compared to other PTES designs. We show how the round-trip efficiency, specific power output, capital cost, and levelized cost of storage (LCOS) depend on parameters such as the pressure ratio, heat exchanger approach temperature and pressure loss, and maximum temperature. We compare particle-PTES (P-PTES) performance to PTES which uses liquid thermal energy storage - i.e. molten salt hot storage and methanol cold storage (MS-PTES). We find that using silica particles for storage advances PTES technology: P-PTES can be operated at higher maximum temperatures than MS-PTES. Furthermore, P-PTES can achieve lower approach temperatures in the heat exchangers than MS-PTES without increasing capital costs, because P-PTES uses direct-contact heat transfer in fluidized bed heat exchangers. As a result, we find that P-PTES systems achieve higher round-trip efficiency than MS-PTES (66 % versus 57 %) and lower LCOS (e.g. 0.115 +- 0.03 $/kWhe versus 0.171 +- 0.04 $/kWhe for 10 h discharge). The low cost of particles and containment means that P-PTES can provide long-duration energy storage at low capital cost per unit energy capacity. For example, the total capital cost per unit energy reduces from 245 $/kWhe at 10 h to 38 $/kWhe at 100 h. These costs are considerably lower than MS-PTES (72 $/kWhe at 100 h) and also outcompete current and future Li-ion battery system projections (100-265 $/kWhe).

25 ENERGY STORAGE↗
DOE OSTI2022

Fast and Simple Ag/Cu Ion Exchange on Cu Foil for Anode-Free Lithium-Metal Batteries

Lithium-metal batteries with zero excess lithium on the anode side paired with a fully lithiated cathode are regarded as a form of the highest energy-density configuration. Unfortunately, the continuous lithium loss over cycling from a limited amount of lithium reservoir significantly degrades the overall cell performance in the anode-free system. To mitigate the deterioration, modifying the current collector for enhanced lithium cycling is an indispensable route. Here, we apply a Ag/Cu ion exchange to precipitate micro-sized Ag particles on the Cu current collector to enhance the lithium reversibility via (de)alloying process. Further, we show a smoother morphology of lithium upon alloying, which leads to a lowered nucleation potential as well as increased average Coulombic efficiency in Li||Cu cells regardless of electrolyte formulation. The preferred lithium adsorption on Ag and AgLi over Cu is demonstrated with density functional theory calculations, which supports that Li is forming a gamma-phase alloy in the last stage rather than being deposited beneath the alloy. Lastly, this simple Cu foil modification enhances lithium reversibility and reduces its nucleation barrier, thus mitigating the capacity fade of a Cu||LiFePO 4 with reduced polarization.

25 ENERGY STORAGE↗
DOE OSTI2023

Enhanced Iodine Capture Using a Postsynthetically Modified Thione–Silver Zeolitic Imidazole Framework

Efficient management of radionuclides that are released from various processes in the nuclear fuel cycle is of significant importance. Among these nuclides, radioactive iodine (mainly 129 I and 131 I) is a major concern due to the risk it poses to the environment and to human health; thus, the development of materials that can capture and safely store radioactive iodine is crucial. Herein, a novel silver-thione-functionalized zeolitic imidazole framework (ZIF) was synthesized via post-synthetic modification and assessed for its iodine uptake capabilities alongside the parent ZIF-8 and intermediate materials. A solvent-assisted ligand exchange procedure was used to replace the 2-methylimidazole linkers in ZIF-8 with 2-mercaptoimidazole, forming the intermediate compound ZIF-8=S, which was reacted with AgNO 3 to yield the ZIF-8=S-Ag + composite for iodine uptake. Despite possessing the lowest BET surface area of the derivatives, the Ag-functionalized material demonstrated superior I 2 adsorption in terms of both maximum capacity (550 g I 2 /mol) and rapid kinetics (50% loading achieved in 5 hrs, saturation in 50 hrs) compared to our pristine ZIF-8, which reached 450 g I 2 /mol after 150 hours and 50% loading in 25 hours. This improvement is attributed to the presence of the Ag + ions, which provide a strong chemical driving force to form stable Ag-I species. In conclusion, the results of this study contribute to a broader understanding of the strategies that can be employed to engineer adsorbents with robust iodine uptake behavior.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A series of cation-modified robust zirconium-based metal–organic frameworks for carbon dioxide capture

Metal–organic frameworks (MOFs) represent one of the most promising porous solids for possible use as sorbents to control and reduce the greenhouse gas emission. Studies have shown that open metal sites (OMS) interact strongly with carbon dioxide and thus, serve as efficient binding sites for CO 2 capture. However, many OMS-bearing MOFs are lack of framework stability and often have high regeneration temperature. To seek ways to solve the stability issue, we designed a series of isoreticular MOFs, Zr-tcpb-COOM (M = alkali/alkaline earth metal), by exchange of protons with metal ions on Zr-tcpb-COOH via post-synthetic modification (PSM). The pristine MOF (Zr-tcpb-COOH) has a very robust framework. The PSM process does not deteriorate the framework stability but creates metal binding sites that form strong bonds with carbon dioxide. The results show that at low CO 2 pressure, the uptake amount is enhanced considerably using Zr-tcpb-COOM and is in trend of increasing atomic number (Li + < Na + < K + < Ca 2+ ). High adsorption selectivity (CO 2 /N 2 IAST selectivity (15 : 85) = 539.5) is also achieved for CO 2 over N 2 at room temperature. This approach offers a feasible method to improve CO 2 capture capacity, especially at low concentrations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Vacancy Control in TiNb 2 O 7 : Implications for Energy Applications

Rapid global electrification, including for transportation, has dramatically increased demand for long-lasting and faster-charging batteries. Titanium niobium oxide (TiNb 2 O 7 ) is one of the most promising anode materials for high-power lithium-ion batteries (LIBs). However, the intrinsic low electronic conductivity of TiNb 2 O 7 is a significant drawback. Herein, an almost 10 orders of magnitude increase in conductivity is achieved via reduction of TiNb 2 O 7 in H 2 at 900 °C. The observed dramatic increase in electron conductivity upon reduction is unprecedented and opens new possibilities to produce niobium-based conductive materials for next-generation energy storage. Upon extended reduction, TiNb 2 O 7 converts into a distorted rutile TiNb 2 O 6 structure, which can be reoxidized back into the crystallographic shear phase. In addition, TiNb 2 O 7 can be thermally reduced in an inert atmosphere and reoxidized by CO 2 with excellent oxygen exchange capacity. Thus, the TiNb 2 O 7 Wadsley–Roth phase demonstrates outstanding potential for solar-driven thermochemical CO 2 splitting at 1400 °C. In conclusion, these findings manifest that controlling defect chemistry paves the way for developing advanced materials for LIBs and solar-driven thermochemical fuel production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Nonlinear magnons and exchange Hamiltonians of the delafossite proximate quantum spin liquid candidates KYbSe 2 and NaYbSe 2

Quantum spin liquids (QSLs) are theoretical states of matter with long-range entanglement and exotic quasiparticles. However, they generally elude quantitative theory, rendering their underlying phases mysterious and hampering efforts to identify experimental QSL states. Here we study triangular-lattice resonating-valence-bond QSL candidate materials KYbSe 2 and NaYbSe 2 . We measure the magnon modes in their 1/3 plateau phase, where quantitative theory is tractable, using inelastic neutron scattering and fit them using nonlinear spin wave theory. We also fit the KYbSe 2 heat capacity using high-temperature series expansion. Both KYbSe 2 fits yield the same magnetic Hamiltonian to within uncertainty, confirming previous estimates and showing the Heisenberg ratio J 2 / J 1 to be an accurate model for these materials. Most importantly, comparing KYbSe 2 and NaYbSe 2 shows that the smaller A -site Na + ion has a larger J 2 / J 1 ratio. However, hydrostatic pressure applied to KYbSe 2 increases the ordering temperature (a result consistent with density functional theory calculations), indicating that pressure decreases J 2 / J 1 . In conclusion, these results show how the periodic table and hydrostatic pressure can tune the A YbSe 2 materials in a controlled way.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Modified Isotherm Modeling to Predict Cs Exchange with Crystalline Silicotitanate in Tank Waste Simulants

The U.S. Department of Energy is working to expedite processing of Hanford tank waste supernate at the Hanford Waste Treatment and Immobilization Plant. To support this goal, Washington River Protection Solutions is designing a Tank Side Cesium Removal (TSCR) system for suspended solids and cesium (Cs/ 137 Cs) removal from Hanford tank waste supernate. The ion exchange media selected for Cs removal at TSCR is crystalline silicotitanate (CST) that is manufactured in a nearly spherical form by Honeywell UOP LLC (UOP; Des Plaines, IL) as product IONSIV® R9140-B (Na form). The Zheng Anthony Miller (ZAM) isotherm model (Zheng et al. 1997) is a multicomponent ion exchange model used to predict the exchange of Group I metals onto CST. The ZAM isotherm has historically been used to predict Cs distribution values from Hanford and Savannah River Site (SRS) tank waste simulants. Figure S.1 summarizes model predictions from the ZAM isotherm that indicate poor prediction of Cs distribution values for simple and complex simulants with the engineered form of CST, IONSIV® R9140-B, and IONSIV® R9120-B where the solid line indicates a perfect fit by the model. The dotted lines indicate ±20% error. Batch contact testing with Hanford tank waste complex and simple simulants was used in conjunction with SRS simulants to experimentally determine Cs distribution values using a modification to the original isotherm model. The experimentally determined maximum Cs capacity for IONSIV® R9140-B CST in both the simple and complex matrices was found to be 0.53±0.3 mmoles Cs/g of CST. This value is not drastically different from the maximum Cs capacity of 0.58 mmoles Cs/g TAM-5 reported by Zheng et al. (1997). However, it is important to note that TAM-5 (commercially IONSIV® IE-910) is a powder. Hamm et al. (2002) determined that a dilution factor was needed to account for the Zr(OH)2 binder in the engineered form of CST. Hamm et al. determined that a dilution factor of 0.68 was appropriate to account for binder contribution and correct overprediction of Cs exchange on the engineered form of CST in ZAM calculations. This reduced the total capacity from 0.58 mmol/g with TAM-5 to 0.39 mmol/g for the engineered form of CST (Hamm et al. 2002). Despite substituting the experimentally determined maximum Cs capacity of 0.55 mmoles Cs/g for the literature-reported capacity of 0.39 mmoles Cs/g, it was determined that additional modifications to the model’s equilibrium rate constants were necessary in refining the isotherm model. The modified model overpredicted K+ uptake by the CST when compared to digested CST results described by Campbell et al. (2019). The modified model was further revised to omit three of the five K+ exchange equilibrium reactions described by ZAM to reduce the additional K+ loading seen by the model. Figure S.2 summarizes the revised model isotherm predictions plotted against measured Kd values.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗