Solid-phase zirconium and fluoride species in alkaline zircaloy cladding waste at Hanford

Reynolds, Jacob G.; Huber, Heinz; Cooke, Gary A.; Pestovich, John A.

doi:10.1016/j.jhazmat.2014.05.097

Cited by 26 publications

(31 citation statements)

References 16 publications

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“…Sodium fluoride salt is frequently present in the Hanford waste. 27 The solubility of NaF in pure water is about 0.987 m at 25 °C. 24 Therefore, the lowest sodium and highest fluoride concentration in Figure 1 is 0.987 m because NaF salt breaks up into one sodium ion and one fluoride ion during dissolution via the following reaction …”

Section: Resultsmentioning

confidence: 99%

Salt Solubilities in Aqueous Solutions of NaNO₃, NaNO₂, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

Reynolds

2018

ACS Omega

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Nonelectrolyte solubility in electrolyte solutions follow the Hofmeister series, but the applicability of the series to salt solubility has been less appreciated. This study, using solubility data for thirteen sodium-bearing salts, shows that salts are consistently salted out by electrolytes important to alkaline nuclear waste in the order NaOH > NaCl > NaNO2 > NaNO3 at 298.15 K, which is the same order as the Hofmeister series. Graphical presentation allowed for easy separation of the common ion effect (caused by the addition of Na+) from the salting-out effect (caused by the presence of anions) because there is a large difference between the solubility of a given salt in different background electrolytes at a common Na+ molality. The trend persists even in very high electrolyte concentrations where essentially all of the water molecules must be in the coordination sphere of an ion, which means that the effect of electrolytes on “bulk water” is not the cause of the trend. These specific interactions more likely result from the sharing of water molecules between ions, augmented by differences in ion-pairing of the electrolytes. The Hofmeister series has practical application to the management of alkaline high-level radioactive waste created at nuclear fuel reprocessing facilities, where a predictive understanding of salt solubility is essential for blending wastes of disparate compositions prior to treatment.

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Section: Resultsmentioning

confidence: 99%

Salt Solubilities in Aqueous Solutions of NaNO₃, NaNO₂, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

Reynolds

2018

ACS Omega

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“…From a nuclear waste management perspective, the present data can be used to estimate the minimum quantity of water required to dissolve NaF from sludge at the Hanford site. For instance, tank 241-AW-103 at the Hanford site has NaF as the dominate salt in the solid phase and is estimated to have 1.15 × 10 5 kg (6.06 × 10 6 moles) of fluoride. , Once the sodium-bearing interstitial liquid is washed out, approximately 6.14 × 10 6 kg of water are required to dissolve the NaF out of this single tank at 25 °C. If the water is evaporated after the NaF is dissolved into it, the NaF will simply reprecipitate.…”

Section: Discussionmentioning

confidence: 99%

“…The present work came out of interest in alkaline nuclear wastes at the Hanford site near Richland, WA, in the United States of America, where NaF as well as NaF-containing double salts have precipitated. , Nuclear wastes are highly concentrated electrolyte solution containing NaNO 2 , NaNO 3 , NaOH, and NaAl(OH) 4 as the most prevalent electrolytes, with many other electrolytes (including fluoride) being present. Given the complexity of the waste, solubility models are being developed − to the support of the remediation effort.…”

Section: Introductionmentioning

confidence: 99%

A Review of Sodium Fluoride Solubility in Water

Reynolds

Belsher

2017

J. Chem. Eng. Data

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The solubility of NaF in water is important to a number of industries, but there is a limited review of the large amount of solubility data scattered throughout the literature. The present study collected all of the data on the NaF solubility in water that could be found in the peer-reviewed literature between the temperature 0 and 100.6 °C (the upper temperature being approximately the boiling point of a saturated solution). Fifty-five solubility data points were found, collected from 29 studies. There was a large amount of scatter among the data, both across and within most studies. After screening out suspect data, the solubility of NaF was found to be a linear function of temperature, with a change of solubility of 0.003 molal per °C. Averaging the data at 25 °C provides an estimated solubility of 0.987 molal at that temperature.

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“…Recently, the interest in natrophosphate has been renewed due to its findings as one of the major salts in alkaline nuclear wastes such as those stored at the Hanford site, near Richland, WA, USA [18][19][20][21]. The occurrence of this phase considerably complicates the waste processing, which necessitates detailed studies of its composition and solubility.…”

Section: Introductionmentioning

confidence: 99%

Natrophosphate, Arctic Mineral and Nuclear Waste Phase: Structure Refinements and Chemical Variability

2021

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The crystal structures of natural (Mt. Koashva, Khibiny alkaline massif, Kola Peninsula, Russian Arctic) and synthetic (obtained from an aqueous solution of sodium phosphate and sodium fluoride (1:1) by evaporation at room temperature (RT)) natrophosphate, Na7(PO4)2F·19H2O, have been investigated using single-crystal X-ray diffraction analysis. Natrophosphate and its synthetic analogue are cubic, Fd-3c, a = 27.6942(3) Å (natrophosphate at RT), a = 27.6241(4) Å (natrophosphate at 100 K), a = 28.1150(12) Å (synthetic analogue at RT), a = 27.9777(7) Å (synthetic analogue at 100 K). The crystal structure is based upon the super-octahedral [Na6(H2O)18F]5+ polycationic complexes consisting of six edge-linked Na6(OH2)5F octahedra sharing one common fluorine vertex. The A site is statistically occupied by Na and H2O with the prevalence of H2O with the refined occupancy factors O:Na equal to 0.53:0.47 for natrophosphate and 0.75:0.25 for its synthetic analogue. The coordination of the A site in synthetic natrophosphate is enlarged compared to the natural sample, which agrees well with its higher occupancy by H2O molecules. The general formula of natrophosphates can be written as Na6+xHxF(PO4)2·(19 + x)H2O, where x = 0–1. The chemical variability of natrophosphate allows to explain the discrepancies in its solubility reported by different authors. The information-based parameters of structural complexity are equal to 3.713 bit/atom and 2109.177 bit/cell that allows to classify natrophosphate as a structurally very complex mineral.

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Solid-phase zirconium and fluoride species in alkaline zircaloy cladding waste at Hanford

Cited by 26 publications

References 16 publications

Salt Solubilities in Aqueous Solutions of NaNO₃, NaNO₂, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

Salt Solubilities in Aqueous Solutions of NaNO₃, NaNO₂, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

A Review of Sodium Fluoride Solubility in Water

Natrophosphate, Arctic Mineral and Nuclear Waste Phase: Structure Refinements and Chemical Variability

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Solid-phase zirconium and fluoride species in alkaline zircaloy cladding waste at Hanford

Cited by 26 publications

References 16 publications

Salt Solubilities in Aqueous Solutions of NaNO3, NaNO2, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

Salt Solubilities in Aqueous Solutions of NaNO3, NaNO2, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

A Review of Sodium Fluoride Solubility in Water

Natrophosphate, Arctic Mineral and Nuclear Waste Phase: Structure Refinements and Chemical Variability

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Salt Solubilities in Aqueous Solutions of NaNO₃, NaNO₂, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste

Salt Solubilities in Aqueous Solutions of NaNO₃, NaNO₂, NaCl, and NaOH: A Hofmeister-like Series for Understanding Alkaline Nuclear Waste