Identification and time evolution of thionyl chloride (SOCl2) radiolysis products
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Jacy K. Conrad
,
Michael E. Woods
and
Gregory P. Horne
Abstract
Innovative solutions are needed to reduce the amount of high-level waste generated by used nuclear fuel recycling strategies to support the widespread adoption of sustainable nuclear fission energy technologies. To this end, a new sulfur chloride-based process has been developed to recycle zirconium alloy-based materials, which make up a significant fraction of high-level radioactive waste. To support the continued development of this process, we present new data on the potential reaction pathways over time of the products arising from the gamma and electron beam radiolysis of neat thionyl chloride (SOCl2). Interrogation of the gamma irradiated liquid by Raman spectroscopy provided more conclusive identification of the SOCl2 degradation products, specifically sulfur dichloride (SCl2), molecular chlorine (Cl2), sulfur dioxide (SO2), and sulfuryl chloride (SO2Cl2). In comparison, the high dose rate (∼107 Gy s−1) electron beam irradiations formed significantly more degradation products. For both cobalt-60 gamma and electron beam irradiations, the observed degradation products were found to evolve as a function of time post-irradiation via the same reaction pathways, with indication of a solvent regeneration mechanism. These findings are fortuitous for process development, as such a mechanism would be beneficial for process longevity and cost effectiveness.
Acknowledgments
The authors would also like to thank Brian L. Berls, Kevin L. Folkman, Chad C. O’Neil, and Jon Stoner for access to IAC beamline facilities and support with electron beam experiments, and graduate students Zoe C. Emory (University of Notre Dame) and Brian M. Rotermund (Colorado School of Mines) for assistance in performing Fricke dosimetry measurements for the electron beam irradiation experiments.
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Research ethics: Not applicable.
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Informed consent: Not applicable.
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Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.
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Competing interests: The authors state no conflict of interest.
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Research funding: This research was funded by the U.S. Department of Energy (DOE) Assistant Secretary for Nuclear Energy, under the Material Recovery and Waste Form Development Campaign, DOE-Idaho Operations Office Contract DE-AC07-05ID14517.
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Data availability: The raw data can be obtained on request from the corresponding author.
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Articles in the same Issue
- Frontmatter
- Original Papers
- Independent isomeric yield ratios of fission products in the epi-cadmium neutron-induced fission of 245Cm
- Preparation of MnO2 modified winter melon-derived biochar for enhanced adsorption of U(VI) from aqueous solution
- Separation studies of 60Co (II) and 134Cs (I) radionuclides from aqueous solution using starch-grafted citric acid-acrylamide/magnesia hydrogel
- Study on the adsorption performance of zeolite imidazole frameworks materials for Co(II) and Mn(II) in solution
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- [113mIn]In-PSMA: high potential agent for SPECT imaging of prostate cancer
- Physicochemical model of uranium hexafluoride (UF6) radiolysis under action of alpha particles
- Identification and time evolution of thionyl chloride (SOCl2) radiolysis products
- Measurement of gross alpha radioactivity levels and estimation of annual effective dose in hazelnut kernels
- Characterization of ferrous-xylenol orange-polyvinyl alcohol gel for gamma dosimetry using spectroscopy
Articles in the same Issue
- Frontmatter
- Original Papers
- Independent isomeric yield ratios of fission products in the epi-cadmium neutron-induced fission of 245Cm
- Preparation of MnO2 modified winter melon-derived biochar for enhanced adsorption of U(VI) from aqueous solution
- Separation studies of 60Co (II) and 134Cs (I) radionuclides from aqueous solution using starch-grafted citric acid-acrylamide/magnesia hydrogel
- Study on the adsorption performance of zeolite imidazole frameworks materials for Co(II) and Mn(II) in solution
- Synthesis, in silico and biodistribution studies of a novel 47Sc-radiolabeled α-amino acid ester derivative attached to pyrazine and tetrazole rings for tumor targeted radiotherapy
- [113mIn]In-PSMA: high potential agent for SPECT imaging of prostate cancer
- Physicochemical model of uranium hexafluoride (UF6) radiolysis under action of alpha particles
- Identification and time evolution of thionyl chloride (SOCl2) radiolysis products
- Measurement of gross alpha radioactivity levels and estimation of annual effective dose in hazelnut kernels
- Characterization of ferrous-xylenol orange-polyvinyl alcohol gel for gamma dosimetry using spectroscopy
