碳酸铀形成前电离辐射对过氧化铀的活化作用

IF 3.5 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Dalton Transactions Pub Date : 2024-09-26 DOI:10.1039/d4dt01841a

Zoe Emory, Peter C Burns, Jay LaVerne

{"title":"碳酸铀形成前电离辐射对过氧化铀的活化作用","authors":"Zoe Emory, Peter C Burns, Jay LaVerne","doi":"10.1039/d4dt01841a","DOIUrl":null,"url":null,"abstract":"The solid form of the uranyl peroxide cage (UPC) cluster LiU28 (Li28[(UO2)28(O2)42]) was irradiated by 5 MeV He2+ ions to achieve doses up to 42 MGy. An intermediate compound formed that reacts with atmospheric CO2 to form uranyl carbonates. The role of water in the UPC to uranyl carbonate transformation was studied by flowing either dry or hydrated Ar over samples during He2+ irradiation, and by storing samples in dry and humid environments before and after irradiation. Raman, infrared, and X-ray photoelectron spectroscopies and electrospray ionization mass spectrometry were used to characterize solid Li-U28 salts before and after He2+ irradiation. The highest yield of uranyl carbonates occurred when hydrated Ar gas was flowed across the sample during He2+ irradiation. Electron paramagnetic resonance spectroscopy provided evidence of hydroxyl and superoxide radicals in both unirradiated and -irradiated Li-U28.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":null,"pages":null},"PeriodicalIF":3.5000,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Activation of uranyl peroxides by ionizing radiation prior to uranyl carbonate formation\",\"authors\":\"Zoe Emory, Peter C Burns, Jay LaVerne\",\"doi\":\"10.1039/d4dt01841a\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The solid form of the uranyl peroxide cage (UPC) cluster LiU28 (Li28[(UO2)28(O2)42]) was irradiated by 5 MeV He2+ ions to achieve doses up to 42 MGy. An intermediate compound formed that reacts with atmospheric CO2 to form uranyl carbonates. The role of water in the UPC to uranyl carbonate transformation was studied by flowing either dry or hydrated Ar over samples during He2+ irradiation, and by storing samples in dry and humid environments before and after irradiation. Raman, infrared, and X-ray photoelectron spectroscopies and electrospray ionization mass spectrometry were used to characterize solid Li-U28 salts before and after He2+ irradiation. The highest yield of uranyl carbonates occurred when hydrated Ar gas was flowed across the sample during He2+ irradiation. Electron paramagnetic resonance spectroscopy provided evidence of hydroxyl and superoxide radicals in both unirradiated and -irradiated Li-U28.\",\"PeriodicalId\":71,\"journal\":{\"name\":\"Dalton Transactions\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2024-09-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Dalton Transactions\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1039/d4dt01841a\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Dalton Transactions","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d4dt01841a","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}

引用次数: 0

摘要

过氧化铀笼（UPC）簇 LiU28（Li28[(UO2)28(O2)42]）的固态形式受到 5 MeV He2+ 离子的辐照，剂量高达 42 MGy。形成的中间化合物与大气中的二氧化碳反应生成铀碳酸盐。通过在氦2+辐照期间将干燥或水合氩流过样品，以及在辐照前后将样品储存在干燥和潮湿的环境中，研究了水在铀化合碳酸铀转化过程中的作用。拉曼光谱、红外光谱和 X 射线光电子能谱以及电喷雾离子化质谱法被用来表征 He2+ 辐照前后的固体 Li-U28 盐。在 He2+ 辐照期间，当水合 Ar 气体流过样品时，铀碳酸盐的产量最高。电子顺磁共振光谱提供了未经辐照和 -irradiated Li-U28 中羟基和超氧自由基的证据。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

Activation of uranyl peroxides by ionizing radiation prior to uranyl carbonate formation

The solid form of the uranyl peroxide cage (UPC) cluster LiU28 (Li28[(UO2)28(O2)42]) was irradiated by 5 MeV He2+ ions to achieve doses up to 42 MGy. An intermediate compound formed that reacts with atmospheric CO2 to form uranyl carbonates. The role of water in the UPC to uranyl carbonate transformation was studied by flowing either dry or hydrated Ar over samples during He2+ irradiation, and by storing samples in dry and humid environments before and after irradiation. Raman, infrared, and X-ray photoelectron spectroscopies and electrospray ionization mass spectrometry were used to characterize solid Li-U28 salts before and after He2+ irradiation. The highest yield of uranyl carbonates occurred when hydrated Ar gas was flowed across the sample during He2+ irradiation. Electron paramagnetic resonance spectroscopy provided evidence of hydroxyl and superoxide radicals in both unirradiated and -irradiated Li-U28.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.