Identification and time evolution of thionyl chloride (SOCl2) radiolysis products

IF 1.4 3区 化学 Q4 CHEMISTRY, INORGANIC & NUCLEAR
Jacy K. Conrad, Michael E. Woods, Gregory P. Horne
{"title":"Identification and time evolution of thionyl chloride (SOCl2) radiolysis products","authors":"Jacy K. Conrad, Michael E. Woods, Gregory P. Horne","doi":"10.1515/ract-2024-0288","DOIUrl":null,"url":null,"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 (SOCl<jats:sub>2</jats:sub>). Interrogation of the gamma irradiated liquid by Raman spectroscopy provided more conclusive identification of the SOCl<jats:sub>2</jats:sub> degradation products, specifically sulfur dichloride (SCl<jats:sub>2</jats:sub>), molecular chlorine (Cl<jats:sub>2</jats:sub>), sulfur dioxide (SO<jats:sub>2</jats:sub>), and sulfuryl chloride (SO<jats:sub>2</jats:sub>Cl<jats:sub>2</jats:sub>). In comparison, the high dose rate (∼10<jats:sup>7</jats:sup> Gy s<jats:sup>−1</jats:sup>) 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.","PeriodicalId":21167,"journal":{"name":"Radiochimica Acta","volume":null,"pages":null},"PeriodicalIF":1.4000,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Radiochimica Acta","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1515/ract-2024-0288","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0

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.
亚硫酰氯(SOCl2)辐射分解产物的鉴定和时间演化
需要创新的解决方案来减少废旧核燃料回收战略产生的高放射性废物量,以支持可持续核裂变能源技术的广泛采用。为此,我们开发了一种基于氯化硫的新工艺,用于回收锆合金材料,这种材料在高放射性废物中占很大比例。为了支持这一工艺的持续发展,我们提供了关于纯净的亚硫酰氯(SOCl2)在伽马射线和电子束辐射分解过程中产生的产物随时间变化的潜在反应途径的新数据。利用拉曼光谱对伽马射线辐照过的液体进行分析,可以更准确地确定 SOCl2 的降解产物,特别是二氯化硫(SCl2)、分子氯(Cl2)、二氧化硫(SO2)和硫酰氯(SO2Cl2)。相比之下,高剂量率(∼107 Gy s-1)电子束辐照产生的降解产物要多得多。在钴-60 伽马辐照和电子束辐照中,观察到的降解产物都是通过相同的反应途径随辐照后时间的变化而变化的,这表明存在溶剂再生机制。这些发现对于工艺开发来说是非常幸运的,因为这种机制将有利于工艺的寿命和成本效益。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Radiochimica Acta
Radiochimica Acta 化学-核科学技术
CiteScore
2.90
自引率
16.70%
发文量
78
审稿时长
6 months
期刊介绍: Radiochimica Acta publishes manuscripts encompassing chemical aspects of nuclear science and technology.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信