Structure and aggregation behavior of pertechnetate/perrhenate in organic phase in the extraction by tributyl phosphate
Abstract The extraction of pertechnetate ($ TcO_{4} $−) and perrhenate ($ ReO_{4} $−) by tributyl phosphate (TBP) has been extensively studied, but the structure of the extracted species is subject to debate. In this work, the extraction behavior of $ TcO_{4} $− and $ ReO_{4} $− from both $ HNO_{3} $ and HCl media by TBP in n-dodecane was studied by examining the effects of acid concentration, extractant concentration, and temperature on the extraction. The two anions displayed similar extraction behavior in both the $ HNO_{3} $ and HCl systems, where the distribution ratio of $ TcO_{4} $− was slightly higher than that of $ ReO_{4} $−. The measurement of water content in the organic phase and dynamic light scattering were carried out, which in combination with the extraction behavior indicated that $ ReO_{4} $− was extracted as [$ H^{+} %$ ReO_{4} $−($ H_{2} $O)8·(TBP)4] and formed microemulsions in the organic phase. Theoretical calculations were performed on the structure of both [$ H^{+} %$ ReO_{4} $−($ H_{2} $O)8·(TBP)4] and [$ H^{+} %$ TcO_{4} $−($ H_{2} $O)8·(TBP)4]. The TBP molecules interacted with the [$ H^{+} %$ ReO_{4} $−($ H_{2} $O)8] and [$ H^{+} %$ TcO_{4} $−($ H_{2} $O)8] clusters through hydrogen bonding between $ H_{2} $O and the O=P groups, i.e., $ ReO_{4} $− and $ TcO_{4} $− underwent outer-sphere coordination with TBP in the organic phase. Results in this work provide valuable insights into the structures of $ ReO_{4} $− and $ TcO_{4} $− extracted into the organic phase by TBP, and also assist in the analysis of $ TcO_{4} $− species in the PUREX process..
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:332 |
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| Enthalten in: |
Journal of radioanalytical and nuclear chemistry - 332(2023), 6 vom: 13. Apr., Seite 1723-1732 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Liu, Haiwang [VerfasserIn] |
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| Links: |
Volltext [lizenzpflichtig] |
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© Akadémiai Kiadó, Budapest, Hungary 2023. Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law. |
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| doi: |
10.1007/s10967-023-08885-6 |
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SPR052423484 |
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| 100 | 1 | |a Liu, Haiwang |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Structure and aggregation behavior of pertechnetate/perrhenate in organic phase in the extraction by tributyl phosphate |
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| 520 | |a Abstract The extraction of pertechnetate ($ TcO_{4} $−) and perrhenate ($ ReO_{4} $−) by tributyl phosphate (TBP) has been extensively studied, but the structure of the extracted species is subject to debate. In this work, the extraction behavior of $ TcO_{4} $− and $ ReO_{4} $− from both $ HNO_{3} $ and HCl media by TBP in n-dodecane was studied by examining the effects of acid concentration, extractant concentration, and temperature on the extraction. The two anions displayed similar extraction behavior in both the $ HNO_{3} $ and HCl systems, where the distribution ratio of $ TcO_{4} $− was slightly higher than that of $ ReO_{4} $−. The measurement of water content in the organic phase and dynamic light scattering were carried out, which in combination with the extraction behavior indicated that $ ReO_{4} $− was extracted as [$ H^{+} %$ ReO_{4} $−($ H_{2} $O)8·(TBP)4] and formed microemulsions in the organic phase. Theoretical calculations were performed on the structure of both [$ H^{+} %$ ReO_{4} $−($ H_{2} $O)8·(TBP)4] and [$ H^{+} %$ TcO_{4} $−($ H_{2} $O)8·(TBP)4]. The TBP molecules interacted with the [$ H^{+} %$ ReO_{4} $−($ H_{2} $O)8] and [$ H^{+} %$ TcO_{4} $−($ H_{2} $O)8] clusters through hydrogen bonding between $ H_{2} $O and the O=P groups, i.e., $ ReO_{4} $− and $ TcO_{4} $− underwent outer-sphere coordination with TBP in the organic phase. Results in this work provide valuable insights into the structures of $ ReO_{4} $− and $ TcO_{4} $− extracted into the organic phase by TBP, and also assist in the analysis of $ TcO_{4} $− species in the PUREX process. | ||
| 650 | 4 | |a Extraction |7 (dpeaa)DE-He213 | |
| 650 | 4 | |a Pertechnetate |7 (dpeaa)DE-He213 | |
| 650 | 4 | |a Perrhenate |7 (dpeaa)DE-He213 | |
| 650 | 4 | |a Tributyl phosphate |7 (dpeaa)DE-He213 | |
| 700 | 1 | |a Zhang, Yangyang |4 aut | |
| 700 | 1 | |a Chen, Zhuoyuan |4 aut | |
| 700 | 1 | |a Zhang, Zhaofei |4 aut | |
| 700 | 1 | |a Cheng, Xinwei |4 aut | |
| 700 | 1 | |a Xu, Chao |4 aut | |
| 700 | 1 | |a Chen, Jing |4 aut | |
| 700 | 1 | |a Wang, Jianchen |4 aut | |
| 700 | 1 | |a Hu, Hanshi |4 aut | |
| 700 | 1 | |a Sun, Taoxiang |0 (orcid)0000-0003-4690-3566 |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t Journal of radioanalytical and nuclear chemistry |d Dordrecht [u.a.] : Springer Science + Business Media B.V., 1968 |g 332(2023), 6 vom: 13. Apr., Seite 1723-1732 |w (DE-627)SPR015147320 |w (DE-600)2017242-4 |x 1588-2780 |7 nnns |
| 773 | 1 | 8 | |g volume:332 |g year:2023 |g number:6 |g day:13 |g month:04 |g pages:1723-1732 |
| 856 | 4 | 0 | |u https://dx.doi.org/10.1007/s10967-023-08885-6 |z lizenzpflichtig |3 Volltext |
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