High temperature UCl3 synthesis in molten salt mixtures via reaction of U metal with iron chlorides

Zhang, Huan; Newton, Matthew; Hamilton, D. Ethan; Simpson, Michael

doi:10.1007/s10967-021-08060-9

Cited by 4 publications

(1 citation statement)

References 12 publications

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“…Commonly reported lanthanide and actinide chlorination pathways for trichloride formation are often conducted under high temperature environments and include the use of hydrochloric acid or chlorine gas as the chlorinating agent, where oxides, sesquioxides, and hydrides have been utilized as reactants. [8][9][10][11][12][13][14][15] Additionally, chlorination via molten salt mixtures, including LiCl-KCl, NaCl-CaCl 2 , and metallic U, has been widely reported and includes chlorinating agents such as BiCl 3 , 16 CdCl 2 , 17 CuCl 2 , 18 FeCl x , 19 NH 4 Cl, 20 and ZnCl 2 . 21,22 UCl 3 synthesis can additionally be accomplished via hydrogen reduction of the tetrachloride.…”

Section: Introductionmentioning

confidence: 99%

In situ synthesis of PuCl₃ and corresponding Raman and density functional theory vibrational modes

Hanson,

Hubley,

Atta‐Fynn

et al. 2023

J Raman Spectroscopy

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The experimental and calculated Raman spectrum of PuCl3 has been reported for the first time. PuCl3 is a primary species found in plutonium metal refinement, specifically in pyrochemical salt processes including multicycle direct oxide reduction, metal chlorination, and electrorefining. As such, Raman signatures of PuCl3 could serve as potential forensic indicators of material process history. A novel technique for synthesizing PuCl3 from the in situ chlorination of plutonium metal with HCl was developed to establish these signatures. Cerium metal surrogates were utilized to ensure optimization of the plutonium experiments and to minimize personnel exposure, and all experiments were carried out in a Raman reaction chamber designed for air‐tight, high vacuum environments. In situ Raman spectroscopy was employed in conjunction with density functional theory (DFT) to investigate the vibrational modes of PuCl3. Associated mixed oxy and hydroxyl phases are also reported. The combined Raman and DFT results have eliminated inconsistencies in Raman mode assignments for the MX3 family of metal chlorides having P63/m symmetry, and IR modes derived from the DFT calculations are additionally presented. The data observed in this study are of potential interest to nuclear forensic analyses, nuclear sample aging, nuclear energy, plutonium processing, and stockpile stewardship.

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Section: Introductionmentioning

confidence: 99%

In situ synthesis of PuCl₃ and corresponding Raman and density functional theory vibrational modes

Hanson,

Hubley,

Atta‐Fynn

et al. 2023

J Raman Spectroscopy

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Development of a scalable method to chlorinate UO2 to UCl3 using ZrCl4

Chamberlain

Simpson

2022

J Radioanal Nucl Chem

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Application of zero resistance ammeter to real time measurement of redox control in molten chloride salts

Hamilton

Gonzalez²,

Simpson³

2022

J Radioanal Nucl Chem

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High temperature UCl3 synthesis in molten salt mixtures via reaction of U metal with iron chlorides

Cited by 4 publications

References 12 publications

In situ synthesis of PuCl₃ and corresponding Raman and density functional theory vibrational modes

In situ synthesis of PuCl₃ and corresponding Raman and density functional theory vibrational modes

Development of a scalable method to chlorinate UO2 to UCl3 using ZrCl4

Application of zero resistance ammeter to real time measurement of redox control in molten chloride salts

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High temperature UCl3 synthesis in molten salt mixtures via reaction of U metal with iron chlorides

Cited by 4 publications

References 12 publications

In situ synthesis of PuCl3 and corresponding Raman and density functional theory vibrational modes

In situ synthesis of PuCl3 and corresponding Raman and density functional theory vibrational modes

Development of a scalable method to chlorinate UO2 to UCl3 using ZrCl4

Application of zero resistance ammeter to real time measurement of redox control in molten chloride salts

Contact Info

Product

Resources

About

In situ synthesis of PuCl₃ and corresponding Raman and density functional theory vibrational modes

In situ synthesis of PuCl₃ and corresponding Raman and density functional theory vibrational modes