吡啶吡唑基配体C8-BPP对硝酸溶液中Am3+和Eu3+的萃取

doi:10.7503/cjcu20170027

高等学校化学学报 ›› 2017, Vol. 38 ›› Issue (8): 1324.doi: 10.7503/cjcu20170027

• 研究论文: 无机化学 • 上一篇下一篇

吡啶吡唑基配体C8-BPP对硝酸溶液中Am³⁺和Eu³⁺的萃取

胡晓阳¹, 苏冬萍^1,2, 李诗萌¹, 王志鹏¹, 张利荣¹, 刘莹¹, 宋莲君¹, 陈志力¹, 丁颂东¹

1. 四川大学化学学院, 成都 610064;
2. 中国核动力研究设计院, 成都 610005

收稿日期:2017-01-13 修回日期:2017-07-05 出版日期:2017-08-10 发布日期:2017-07-05
通讯作者: 丁颂东,男,博士,研究员,博士生导师,主要从事核燃料循环与材料研究.E-mail:dsd68@163.com E-mail:dsd68@163.com
基金资助:
国家自然科学基金（批准号：11675115，91426302，91126016）资助.

Extraction of Am(Ⅲ) and Eu(Ⅲ) from Nitric Acid Solution with the Pyridylpyrazole Based Ligand C8-BPP

HU Xiaoyang¹, SU Dongping^1,2, LI Shimeng¹, WANG Zhipeng¹, ZHANG Lirong¹, LIU Ying¹, SONG Lianjun¹, CHEN Zhili¹, DING Songdong¹

1. College of Chemistry, Sichuan University, Chengdu 610064, China;
2. Nuclear Power Institute of China, Chengdu 610005, China

Received:2017-01-13 Revised:2017-07-05 Online:2017-08-10 Published:2017-07-05
Supported by:
Supported by the National Natural Science Foundation of China(Nos.11675115, 91426302, 91126016).

摘要/Abstract

摘要：

合成了吡啶吡唑基配体C8-BPP[2，6-bis（5-（n-octyl）-1H-pyrazol-3-yl）pyridine]，并采用红外光谱、核磁共振波谱、质谱等手段对其进行了表征.以正十二烷为稀释剂，2-溴己酸为协萃剂，研究了C8-BPP从HNO₃溶液中萃取Am³⁺和Eu³⁺的行为.重点考察了萃取时间、酸度和萃取剂浓度等对分配比D和分离因子SF_Am/Eu的影响.在HNO₃浓度为0.2~1.0 mol/L时，C8-BPP萃取Am³⁺和Eu³⁺的D值随HNO₃浓度增加而减小，SF_Am/Eu值先增大后减小；HNO₃浓度为0.5 mol/L时，SF_Am/Eu达到55.随着配体浓度的增加，C8-BPP萃取Am³⁺和Eu³⁺的D值均增加，SF_Am/Eu值缓慢减小，但仍在40以上.斜率分析表明，C8-BPP萃取Am³⁺和Eu³⁺均形成了1： 1型的萃合物.还采用紫外滴定、高分辨质谱、红外光谱、拉曼光谱和时间分辨荧光光谱等方法研究了C8-BPP与Eu³⁺的配位化学行为，并得到了配合物的组成和稳定常数.

关键词: 吡啶吡唑基配体, 溶剂萃取, 镅, 铕, 分离

Abstract:

Pyridylpyrazole based ligand 2,6-bis[5-(n-octyl)-1H-pyrazol-3-yl] pyridine(C8-BPP) was synthesized and characterized by means of mass spectrometry(MS), nuclear magnetic resonance(NMR) spectrometry, and Fourier transform infrared spectrometry(FTIR). In the presence of 2-bromohexanoic acid, using n-dodecane as diluent, the extraction behaviors of Am³⁺ and Eu³⁺ with C8-BPP were investigated. Influences of diluent, contact time, acidity and the ligand concentration on the extraction of Am³⁺ and Eu³⁺ were evaluated in HNO₃ solution. The distribution ratio values of Am³⁺ and Eu³⁺ decreased with increasing HNO₃ concentration from 0.2 to 1.0 mol/L, and increased with increasing ligand concentration from 0.01 to 0.1 mol/L. With the increase of acidity, the separation factors(SF_Am/Eu) increased firstly and then decreased. The maximum value of SF_Am/Eu can reach 55 at 0.5 mol/L HNO₃. Meanwhile, SF_Am/Eu values decreased slowly with increasing the ligand concentration but all the SF_Am/Eu values were above 40. The extraction results also showed that C8-BPP exhibited good selective extraction ability for Am³⁺ over RE³⁺. Moreover, slope analyses indicated the formation of 1:1 complexes of C8-BPP with Am³⁺ and Eu³⁺, separately. Besides, the complexation behaviors of C8-BPP with Eu³⁺ were also investigated by means of UV-Vis spectrometry titration, electrospray ionization mass spectrometry(ESI-MS), FTIR, Raman spectrometry and time-resolved laser-induced fluorescence spectroscopy(TRLFS). The composition and stability constant(lgK) of the complex of C8-BPP with Eu³⁺ were also obtained.

Key words: Pyridylpyrazole based ligand, Solvent extraction, Americium, Europium, Separation

中图分类号:

O615.11

TrendMD:

胡晓阳, 苏冬萍, 李诗萌, 王志鹏, 张利荣, 刘莹, 宋莲君, 陈志力, 丁颂东. 吡啶吡唑基配体C8-BPP对硝酸溶液中Am³⁺和Eu³⁺的萃取. 高等学校化学学报, 2017, 38(8): 1324.

HU Xiaoyang, SU Dongping, LI Shimeng, WANG Zhipeng, ZHANG Lirong, LIU Ying, SONG Lianjun, CHEN Zhili, DING Songdong. Extraction of Am(Ⅲ) and Eu(Ⅲ) from Nitric Acid Solution with the Pyridylpyrazole Based Ligand C8-BPP. Chem. J. Chinese Universities, 2017, 38(8): 1324.

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吡啶吡唑基配体C8-BPP对硝酸溶液中Am³⁺和Eu³⁺的萃取

Extraction of Am(Ⅲ) and Eu(Ⅲ) from Nitric Acid Solution with the Pyridylpyrazole Based Ligand C8-BPP

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