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Structural Characterization of Ternary Salt Melts for Low Activity Waste Applications

Published online by Cambridge University Press:  21 February 2019

Emily Nienhuis ,
Muad Saleh Open the ORCID record for Muad Saleh [Opens in a new window]  and
John McCloy Open the ORCID record for John McCloy [Opens in a new window]
Emily Nienhuis*
Affiliation:
Washington State University, Materials Science and Engineering Program
Muad Saleh
Affiliation:
Washington State University, Materials Science and Engineering Program
John McCloy
Affiliation:
Washington State University, Materials Science and Engineering Program Washington State University, School of Mechanical and Materials Engineering
*
*(Email: [email protected])
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Abstract

Reactions of alkali salts (nitrates, sulfates, carbonates, halides, borates) play a key role in the low temperature feed conversion occurring at the cold cap during processing of Hanford Low Activity Waste (LAW) glass melters. An alkali salt phase can sometimes form, and preferentially incorporate radionuclides of Cs, Cl, I, and Tc. During melting of the slurry feed, some of the feed components sequentially break down with increasing temperature to form gases (i.e., nitrates ➔ NOx, carbonates ➔ CO2, and boric acid ➔ H2O) or partially volatilize (halides). Sulfate, however, tends not to volatilize but has limited solubility in the final borosilicate glass waste form. To improve understanding of these low temperature processes and their composition dependencies, a scoping study was undertaken to synthesize salt systems that remain amorphous at room temperature, thus facilitating structural study. Melts of equimolar ratios of K2SO4-ZnSO4 (a known ionic glass-forming system) with added nitrates, halides, or carbonates, were melted and quenched. Some of the materials formed single phase glasses and some underwent crystallization upon quenching. Characterization of these quenched materials by thermal analysis, infrared absorption, and diffraction was performed. Addition of other anions to the sulfate base glass resulted in a distortion of the sulfate tetrahedron, as evidenced by infrared absorption. Carbonates strongly promoted crystallization, mostly of carbonate phases. Nitrates promoted crystallization of ZnO, and the nitrate volatilized with some incorporating into the glass. Halides tended to incorporate into the glass, but the small (F) and large (I) halogens promoted crystallization of sulfate-containing crystals, while moderate sized (Cl) halogens produced single-phase ionic glasses.

Keywords

glassx-ray diffraction (XRD)infrared (IR) spectroscopy
Type
Articles
Information
MRS Advances , Volume 4 , Issue 17-18: Energy-Transfer, Storage and Conversion , 2019 , pp. 1045 - 1056
Copyright
Copyright © Materials Research Society 2019 

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