Dehalogenation of electrochemical processing salt simulants with ammonium phosphates and immobilization of salt cations in an iron phosphate glass waste form

Riley, Brian J.; Peterson, James M.; Vienna, John D.; Ebert, W. L.; Frank, S. M.

doi:10.1016/j.jnucmat.2019.151949

Cited by 21 publications

(53 citation statements)

References 26 publications

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“…The US DOE scientists have recently developed a method to dehalogenate the chloride-rich salt waste using ammonium dihydrogen phosphate (NH 4 H 2 PO 4 ). 42 The reaction between metal chlorides and NH 4 H 2 PO 4 proceeds at 200 • C-600…”

Section: Implications Of Study On the Vitrification Of Phosphate-rich Dehalogenated Electrochemical (Echem) Salt Wastementioning

confidence: 99%

“…A detailed description of the above-mentioned process has been reported elsewhere. 42 The baseline DOE plan is to convert the as-produced alkali phosphate glass into a durable alkali iron phosphate glassy waste form. However, owing to the poor thermal stability of alkali-rich iron phosphate glasses, 43 the majority of potential glassy waste forms developed by the DOE scientists exhibit high tendency toward devitrification (upon cooling of melt) of alkali iron phosphate-based phases, for example, LiFeP 2 O 7 , KFeP 2 O 7 , Li 3 Fe 2 P 3 O 12 , and Na 3 Fe 3 (PO 4 ) 4 , thus, resulting in poor chemical durability.…”

Section: Implications Of Study On the Vitrification Of Phosphate-rich Dehalogenated Electrochemical (Echem) Salt Wastementioning

confidence: 99%

“…However, owing to the poor thermal stability of alkali-rich iron phosphate glasses, 43 the majority of potential glassy waste forms developed by the DOE scientists exhibit high tendency toward devitrification (upon cooling of melt) of alkali iron phosphate-based phases, for example, LiFeP 2 O 7 , KFeP 2 O 7 , Li 3 Fe 2 P 3 O 12 , and Na 3 Fe 3 (PO 4 ) 4 , thus, resulting in poor chemical durability. 42,44 This makes the current formulation of iron phosphate glass unlikely candidates for storage in steel canisters. Another major challenge with iron phosphate glassy waste forms is expected to be their processing in the existing US melter infrastructure.…”

Section: Implications Of Study On the Vitrification Of Phosphate-rich Dehalogenated Electrochemical (Echem) Salt Wastementioning

confidence: 99%

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Structural dependence of crystallization in phosphorus‐containing sodium aluminoborosilicate glasses

Ping

Kapoor²,

Kobera

et al. 2021

J Am Ceram Soc.

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The article reports on the structural dependence of crystallization in Na 2 O-Al 2 O 3 -B 2 O 3 -P 2 O 5 -SiO 2 -based glasses over a broad compositional space. The structure of melt-quenched glasses has been investigated using 11 B, 27 Al, 29 Si, and 31 P magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy, while the crystallization behavior has been followed using X-ray diffraction and scanning electron microscopy combined with energy dispersive spectroscopy. In general, the integration of phosphate into the sodium aluminoborosilicate network is mainly accomplished via the formation of Al-O-P and B-O-P linkages with the possibility of formation of Si-O-P linkages playing only a minor role. In terms of crystallization, at low concentrations (≤5 mol.%), P 2 O 5 promotes the crystallization of nepheline (NaAlSiO 4 ), while at higher concentrations (≥10 mol.%), it tends to suppress (completely or incompletely depending on the glass chemistry) the crystallization in glasses. When correlating the structure of glasses with their crystallization behavior, the MAS NMR results highlight the importance of the substitution/replacement of Si-O-Al linkages by Al-O-P, Si-O-B, and B-O-P linkages in the suppression of nepheline crystallization in glasses. The results have been discussed in the context of (1) the problem of nepheline crystallization in Hanford high-level waste glasses and (2) designing vitreous waste forms for the immobilization of phosphate-rich dehalogenated Echem salt waste.

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Section: Implications Of Study On the Vitrification Of Phosphate-rich Dehalogenated Electrochemical (Echem) Salt Wastementioning

confidence: 99%

Section: Implications Of Study On the Vitrification Of Phosphate-rich Dehalogenated Electrochemical (Echem) Salt Wastementioning

confidence: 99%

Section: Implications Of Study On the Vitrification Of Phosphate-rich Dehalogenated Electrochemical (Echem) Salt Wastementioning

confidence: 99%

See 1 more Smart Citation

Structural dependence of crystallization in phosphorus‐containing sodium aluminoborosilicate glasses

Ping

Kapoor²,

Kobera

et al. 2021

J Am Ceram Soc.

View full text Add to dashboard Cite

show abstract

“…Alternative waste forms for the fission products have also been studied. These alternatives, including silica-alumina-phosphate (SAP) composite and Fe-P-O (iron phosphate) glass waste forms, have been studied to reduce the amount, or improve the durability, of the fission product waste form, and enable reuse of the chlorine in the salt (Frank et al 2015, Riley et al 2019.…”

Section: Waste Salt Glass-bonded Sodalite Ceramic Waste Form Subsystemmentioning

confidence: 99%

Requirements and Conceptual Design of Off-gas Systems for the Reprocessing of Metallic Fuels

Bruffey

Soelberg

Martin

et al. 2020

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An assessment has been conducted to determine how key regulations regarding volatile radionuclide emissions to the atmosphere may apply to the off-gas streams associated with electrochemical reprocessing. The scope of this assessment was based upon a generic electrochemical reprocessing scheme with a throughput rate of 200 MTIHM/y applied to metallic fuel discharged from a sodium fast reactor (SFR), but the findings are able to be translated to other advanced nuclear scenarios as merited. Air dispersion modeling was performed using the EPA CAP-88 model and evaluated the uncontrolled decontamination factors (DFs) that would be required to achieve regulatory compliance with the dosebased limits set forth by EPA regulation 40 CFR 190.10(a). These DFs were compared to those required by fuel cycle-based limits set forth by EPA regulation 40 CFR 190.10(b). Two theoretical sites with disparate climatological conditions were selected for air dispersion modeling (Idaho and Tennessee). Requirements and Conceptual Design of Off-gas Systems for the Reprocessing of Metallic Fuels

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“…Separation processes include selective reaction and/or removal of different salt components such as halides, alkalis, alkaline earths, or rare earths (REs). Salt separation techniques discussed herein include vacuum distillation, melt crystallization, reactive precipitation, oxidative precipitation, zone freezing, and dehalogenation. , The ideal scenario for salt recycle would be a technique for removing the base salt from the fission products, such as distillation or selective crystallization so that (1) the base salt could be recycled for future fuel dissolution batches and (2) only the remaining fission products would need to be immobilized in a wasteform. If this were the case, the wasteform volumes could be significantly reduced compared to waste processing strategies that require the entire salt to be immobilized.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Salt Wasteform Development: A Review of Salt Treatment and Immobilization Options

Riley

2020

Ind. Eng. Chem. Res.

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Electrochemical reprocessing, also referred to as pyroprocessing, is a technique for recycling actinides from used nuclear fuel (UNF) to produce fuel for future reactors. Here, UNF is dissolved in a molten salt (e.g., LiCl-KCl eutectic) within an electrorefiner. After UNF dissolution, fission products are released into the electrolyte salt and converted to chlorides. This paper discusses wasteform options for processing the base electrolyte salt with the fission product salts as well as only the rare-earth (RE) fission products (as RECl3, REOCl, or REO x ) with the intent of finding optimal methods for reducing total waste salt volumes by partitioning the salt for alternate wasteform options. Two of the more detailed partitioning options discussed herein include halide removal from the salt (dehalogenation), which accounts for more than half of the salt on a molar basis, and RE fission product removal for wasteforms with high-RE loadings. Wasteform properties are compared with emphasis on wasteform volume starting from a given amount of (1) total salt cations or (2) RE cations. Comparisons are also made of wasteform chemical durabilities, with the data available from like testing methods. A main conclusion from this work is the justification of subsequent salt processing after electrorefiner operations for achieving significant wasteform volume reduction.

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Dehalogenation of electrochemical processing salt simulants with ammonium phosphates and immobilization of salt cations in an iron phosphate glass waste form

Cited by 21 publications

References 26 publications

Structural dependence of crystallization in phosphorus‐containing sodium aluminoborosilicate glasses

Structural dependence of crystallization in phosphorus‐containing sodium aluminoborosilicate glasses

Requirements and Conceptual Design of Off-gas Systems for the Reprocessing of Metallic Fuels

Electrochemical Salt Wasteform Development: A Review of Salt Treatment and Immobilization Options

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