{"title":"双琥珀酰胺配体选择性分离 Am(III)/Eu(III) 的理论研究","authors":"Peng Ren, Chen-Peng Guan, Hao-Liang Chen, Pin-Wen Huang, Hua-Wu Pei, Ming Qi","doi":"10.1007/s10967-024-09714-0","DOIUrl":null,"url":null,"abstract":"<p>The selective separation of Am(III) over Eu(III) from high-level radioactive liquid waste using four bis-succinamide ligands (THE-BisSCA, L<sup>1</sup>; THDM-BisSCA, L<sup>2</sup>; THDPh-BisSCA, L<sup>3</sup>; THD<sup><i>i−</i></sup>P-BisSCA, L<sup>4</sup>) was explored with density functional theory. Ligands with phenyl groups near the nitrogen, particularly L<sup>3</sup>, showed the highest Eu(III) affinity. The π bonds orbitals of the benzene ring may conjugate with the long pair N-2p orbital, and this special p-π conjugation effect can lead to charge transfer from benzene ring to the donor N atoms on L<sup>3</sup> ligand, resulting a lower energy and more stable structure of the complex formed with the L<sup>3</sup> ligand compared to other complexes. Thermodynamic analysis corroborates L<sup>3</sup> has Eu(III) preference, offering valuable guidance for efficient Am(III) and Eu(III) separation with these ligands.</p>","PeriodicalId":661,"journal":{"name":"Journal of Radioanalytical and Nuclear Chemistry","volume":null,"pages":null},"PeriodicalIF":1.5000,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Theoretical investigation the selective separation of Am(III)/Eu(III) by bis-succinamides ligands\",\"authors\":\"Peng Ren, Chen-Peng Guan, Hao-Liang Chen, Pin-Wen Huang, Hua-Wu Pei, Ming Qi\",\"doi\":\"10.1007/s10967-024-09714-0\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The selective separation of Am(III) over Eu(III) from high-level radioactive liquid waste using four bis-succinamide ligands (THE-BisSCA, L<sup>1</sup>; THDM-BisSCA, L<sup>2</sup>; THDPh-BisSCA, L<sup>3</sup>; THD<sup><i>i−</i></sup>P-BisSCA, L<sup>4</sup>) was explored with density functional theory. Ligands with phenyl groups near the nitrogen, particularly L<sup>3</sup>, showed the highest Eu(III) affinity. The π bonds orbitals of the benzene ring may conjugate with the long pair N-2p orbital, and this special p-π conjugation effect can lead to charge transfer from benzene ring to the donor N atoms on L<sup>3</sup> ligand, resulting a lower energy and more stable structure of the complex formed with the L<sup>3</sup> ligand compared to other complexes. Thermodynamic analysis corroborates L<sup>3</sup> has Eu(III) preference, offering valuable guidance for efficient Am(III) and Eu(III) separation with these ligands.</p>\",\"PeriodicalId\":661,\"journal\":{\"name\":\"Journal of Radioanalytical and Nuclear Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":1.5000,\"publicationDate\":\"2024-08-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Radioanalytical and Nuclear Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1007/s10967-024-09714-0\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Radioanalytical and Nuclear Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1007/s10967-024-09714-0","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
Theoretical investigation the selective separation of Am(III)/Eu(III) by bis-succinamides ligands
The selective separation of Am(III) over Eu(III) from high-level radioactive liquid waste using four bis-succinamide ligands (THE-BisSCA, L1; THDM-BisSCA, L2; THDPh-BisSCA, L3; THDi−P-BisSCA, L4) was explored with density functional theory. Ligands with phenyl groups near the nitrogen, particularly L3, showed the highest Eu(III) affinity. The π bonds orbitals of the benzene ring may conjugate with the long pair N-2p orbital, and this special p-π conjugation effect can lead to charge transfer from benzene ring to the donor N atoms on L3 ligand, resulting a lower energy and more stable structure of the complex formed with the L3 ligand compared to other complexes. Thermodynamic analysis corroborates L3 has Eu(III) preference, offering valuable guidance for efficient Am(III) and Eu(III) separation with these ligands.
期刊介绍:
An international periodical publishing original papers, letters, review papers and short communications on nuclear chemistry. The subjects covered include: Nuclear chemistry, Radiochemistry, Radiation chemistry, Radiobiological chemistry, Environmental radiochemistry, Production and control of radioisotopes and labelled compounds, Nuclear power plant chemistry, Nuclear fuel chemistry, Radioanalytical chemistry, Radiation detection and measurement, Nuclear instrumentation and automation, etc.