γ辐射下CMPO/[C2mim][NTf2]的辐解及其对Eu3+萃取的影响

doi:10.3866/PKU.WHXB201604146

物理化学学报 >> 2016, Vol. 32 >> Issue (8): 2101-2107.doi: 10.3866/PKU.WHXB201604146

γ辐射下CMPO/[C₂mim][NTf₂]的辐解及其对Eu³⁺萃取的影响

袁威津^1,²,董珍^1,²,赵龙^1,^2,*(),于天麟³,翟茂林³

¹ 湖北科技学院非动力核技术研究中心,湖北咸宁437100
² 上海交通大学核科学与工程学院,上海200240
³ 北京大学化学与分子工程学院,北京分子科学国家实验室,北京100871

收稿日期:2016-03-08 发布日期:2016-07-29
通讯作者: 赵龙 E-mail:ryuuchou@sjtu.edu.cn; ryuuchou@hotmail.com
基金资助:
国家自然科学基金(11475112);湖北省2011非动力核技术协同创新计划项目资助

γ-Ray-Induced Radiolysis of CMPO/[C₂mim][NTf₂] and Its Effect on Eu³⁺ Extraction

Wei-Jin YUAN^1,²,Zhen DONG^1,²,Long ZHAO^1,^2,*(),Tian-Lin YU³,Mao-Lin ZHAI³

¹ Non-power Nuclear Technology Research & Development Center, Hubei University of Science & Technology, Xianning 437100, Hubei Province, P. R. China
² School of Nuclear Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China
³ Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China

Received:2016-03-08 Published:2016-07-29
Contact: Long ZHAO E-mail:ryuuchou@sjtu.edu.cn; ryuuchou@hotmail.com
Supported by:
the National Natural Science Foundation of China(11475112);Hubei 2011 Non-power Nuclear Technology Collaborative Innovation Plan, China

摘要/Abstract

摘要：

主要考察了辛基(苯基)-N, N-二异丁基胺甲酰基甲基氧化膦(CMPO)在1-乙基-3-甲基咪唑双三氟甲基磺酰胺酸盐([C₂mim][NTf₂])中的γ辐解行为，同时考察辐射对CMPO/[C₂mim][NTf₂]萃取能力的影响。通过超高效液相色谱-四极杆飞行时间质谱联用仪(UPLC/Q-TOF-MS)进行定量分析、辐解产物认定以及产物半定量分析。CMPO/正十二烷作为对比条件进行了相同研究。结果表明：CMPO在[C₂mim][NTf₂]中的辐解率低于其在正十二烷中，并且辐解路径不同。在正十二烷体系中，CMPO主要发生C―P、C―N键的断链，而在离子液体体系中CMPO主要发生异丁基脱除反应，并与[C₂mim]^+·、·CF₃等离子液体产生的自由基发生取代反应。综合辐解研究结果，我们提出CMPO/[C₂mim][NTf₂]的辐解路径，这加深了CMPO在离子液体中辐解机理的认识。最后，通过萃取实验发现，当硝酸浓度为0.01 mol·L^-1，辐照剂量为800 kGy时，CMPO/[C₂mim][NTf₂]对Eu³⁺的萃取率依旧达到99%以上。

关键词: CMPO, 离子液体, 萃取, 辐解研究, 半定量分析

Abstract:

Theγ-radiolysis of octylphenyl-(N, N-(diisobutyl)carbamoyl-methyl) phosphine oxide (CMPO) in 1-ethyl-3-methylimidazoliumbis (trifluoromethylsulfonyl) imide ([C₂mim][NTf₂]) was studied. The effect of radiation on CMPO/[C₂mim][NTf₂] extractability was also investigated. Quantitative analysis of CMPO in irradiated CMPO/ [C₂mim][NTf₂] systems, identification and semi-quantitative analysis of the radiolytic products were performed using ultra-performance liquid chromatography/quadrupole time-of-flight mass spectrometry (UPLC/Q-TOF-MS). For comparison, CMPO/dodecane was also studied under the same conditions. The radiolysis ratio of CMPO in [C₂mim][NTf₂] was found to be lower than in dodecane, because of the different radiolysis pathways. The radiolysis pathway of CMPO in molecular solvent was mainly chain scission of C―P and C―N, while that in [C₂mim][NTf₂] was the elimination of isobutyl, as well as substitution reactions with [C₂mim]^+· and ·CF₃ generated from solvent [C₂mim][NTf₂]. Based on the radiolysis study, we propose a radiolysis pathway for CMPO/[C₂mim] [NTf₂], providing a deeper understanding of the radiolytic mechanism of CMPO in ionic liquids. Finally, the Eu³⁺ partitioning of CMPO/[C₂mim][NTf₂] from 0.01 mol·L^-1 HNO3 was higher than 99% at 800 kGy.

Key words: CMPO, Ionic liquid, Extraction, Radiolysis study, Semi-quantitative analysis

袁威津,董珍,赵龙,于天麟,翟茂林. γ辐射下CMPO/[C₂mim][NTf₂]的辐解及其对Eu³⁺萃取的影响[J]. 物理化学学报, 2016, 32(8), 2101-2107. doi: 10.3866/PKU.WHXB201604146

Wei-Jin YUAN,Zhen DONG,Long ZHAO,Tian-Lin YU,Mao-Lin ZHAI. γ-Ray-Induced Radiolysis of CMPO/[C₂mim][NTf₂] and Its Effect on Eu³⁺ Extraction[J]. Acta Phys. -Chim. Sin. 2016, 32(8), 2101-2107. doi: 10.3866/PKU.WHXB201604146

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201604146

https://www.whxb.pku.edu.cn/CN/Y2016/V32/I8/2101

参考文献

1	Groenewold G. S. ; Elias G. ; Mincher B. J. ; Mezyk S. P. ; Laverne J. A Talanta 2012, 99 (18), 909.
2	Wei Y. Z Prog. Chem 2011, 23 (7), 1272.
2	韦悦周. 化学进展, 2011, 23 (7), 1272.
3	Nash K. L. ; Gatrone R. C. ; Clark G. A. ; Horwitz P. G. R Sep. Sci. Technol 1988, 23 (12), 1355.
4	Yuan W. J. ; Ao Y. Y. ; Zhao L. ; Zhai M. L. ; Peng J. ; Li J. Q RSC Adv 2014, 4 (93), 51330.
5	Wang S. J. ; Ao Y. Y. ; Zhou H. Y. ; Yuan L. Y. ; Peng J. ; Zhai M. L Acta Phys.-Chim. Sin 2014, 30 (9), 1597.
5	王硕珏; 敖银勇; 周瀚洋; 袁立永; 彭静; 翟茂林. 物理化学学报, 2014, 30 (9), 1597.
6	Yuan L. Y. ; Peng J. ; Xu L. ; Zhai M. L. ; Li J. Q. ; Wei G. S. J. Phys. Chem. B 2009, 113 (26), 8948.
7	Baba Y. ; Kubota F. ; Kamiya N. ; Goto M. J Chem. Eng. Jpn 2011, 44 (10), 679.
8	Ao Y. Y. ; Peng J. ; Yuan L. Y. ; Cui Z. P. ; Cheng L. ; Li J. Q. ; Zhai M. L Dalton Trans 2013, 42 (12), 4299.
9	Yuan W. J. ; Ao Y. Y. ; Zhao L. ; Wei Y. Z. ; Zhai M. L. ; Li J Q. Nucl. Sci. Technol 2015, 26 (1), S10306.
9	袁威津; 敖银勇; 赵龙; 韦悦周; 翟茂林; 李久强. 核科学与技术, 2015, 26 (1), S10306.
10	Ao Y. Y. ; Zhou H. Y. ; Yuan W. J. ; Wang S. J. ; Peng J. ; Zhai M. L. ; Wang J. Y. ; Zhao Z. Q. ; Zhao L. ; Wei Y. Z Dalton Trans 2014, 43 (14), 5580.
11	Shkrob I. A. ; Chemerisov S. D. ; Wishart J. F. J. Phys. Chem. B 2007, 111 (40), 11786.
12	Shkrob I. A. ; Marin T.W. ; Chemerisov S. D. ; Wishart J. F. J. Phys. Chem. B 2011, 115 (37), 10927.
13	Shkrob I. A. J. Phys. Chem. B 2010, 114 (1), 368.
14	Le R. G. ; Lamouroux C. ; Dauvois V. ; Dannoux A. ; Legand S. ; Durand D. ; Moisy P. ; Moutiers G Dalton Trans 2009, No.31, 6175.
15	Yuan L. ; Peng J. ; Xu L. ; Zhai M. ; Li J. ; Wei G. J. Phys. Chem. B 2009, 113 (26), 8948.
16	Dietz M. L. ; Dzielawa J. A. ; Laszak I. ; Young B. A. ; Jensen M. P Green Chem 2003, 5 (6), 682.
17	Visser A. E. ; Swatloski R. P. ; Reichert W. M. ; Griffin S. T. ; Rogers R. D Ind. Eng. Chem. Res 2000, 39 (10), 3596.

[1]	王欢, 吴云雁, 赵燕飞, 刘志敏. 离子液体介导CO₂化学转化研究进展[J]. 物理化学学报, 2021, 37(5): 2010022 - .
[2]	陈文琼, 关永吉, 张姣, 裴俊捷, 张晓萍, 邓友全. 外电场作用下离子液体振动光谱变化的分子动力学模拟研究[J]. 物理化学学报, 2021, 37(10): 2001004 - .
[3]	吴智伟, 丁伟璐, 张雅琴, 王艳磊, 何宏艳. 咪唑类离子液体与酪氨酸相互作用及机理的密度泛函理论研究[J]. 物理化学学报, 2021, 37(10): 2002021 - .
[4]	刘璐, 徐玉萍, 陈霞, 洪梅, 佟静. 1-烷基-3-甲基咪唑氯化物焓变的热重分析[J]. 物理化学学报, 2020, 36(11): 2004014 - .
[5]	惠淑荣, 赵丽薇, 刘青山, 宋大勇. [C₃mim][NTf₂]/DEC/[Li][NTf₂]体系的基础性质[J]. 物理化学学报, 2020, 36(11): 1910067 - .
[6]	胡益民, 韩杰, 郭荣. 非离子表面活性剂Brij 30诱导离子液体型表面活性剂C₁₆imC₈Br蠕虫状胶束向凝胶的转变[J]. 物理化学学报, 2020, 36(10): 1909049 - .
[7]	杨康,帅骁睿,杨化超,严建华,岑可法. 基于室温离子液体的活化石墨烯粉末超级电容储能性能[J]. 物理化学学报, 2019, 35(7): 755 -765 .
[8]	潘明光,赵永升,曾小勤,邹建新. 偶氮苯基型离子液体溶液对空气中湿度的变色响应[J]. 物理化学学报, 2019, 35(6): 624 -629 .
[9]	龚燕燕,刘海春,张朵,佟静. 醚基功能化离子液体[MOEMIm]Cl和[EOEMIm]Cl热力学性质[J]. 物理化学学报, 2019, 35(11): 1224 -1231 .
[10]	陈文琼,关永吉,张晓萍,邓友全. 分子动力学模拟研究外电场对咪唑类离子液体振动谱的影响[J]. 物理化学学报, 2018, 34(8): 912 -919 .
[11]	胡之楠,左剑涛,夏美晨,房大维,臧树良. Pitzer方程应用于离子液体[C_nmim][H₂PO₄](n= 3, 4, 5, 6)溶解焓研究[J]. 物理化学学报, 2018, 34(8): 933 -937 .
[12]	宁汇,王文行,毛勤虎,郑诗瑞,杨中学,赵青山,吴明铂. 1-辛基-3-甲基咪唑功能化石墨片负载氧化亚铜催化二氧化碳电还原制乙烯[J]. 物理化学学报, 2018, 34(8): 938 -944 .
[13]	陈必华,ELAGEED Elnazeer H. M.,张永亚,高国华. 离子液体BmmimOAc催化2-芳氨基乙醇与二硫化碳一步缩合合成3-芳基-2-噻唑硫酮[J]. 物理化学学报, 2018, 34(8): 952 -958 .
[14]	佟静,屈晔,井立强,刘璐,刘春辉. 用恒温热重法测定1-己基-3-甲基咪唑苏氨酸离子液体[C₆mim][Thr]蒸汽压和蒸发焓[J]. 物理化学学报, 2018, 34(2): 194 -200 .
[15]	崔鹏,刘海,于雪敏,夏青,李青松. 水-环己酮-甲基异丁基酮液液相平衡数据的测定与关联[J]. 物理化学学报, 2018, 34(1): 65 -72 .

γ辐射下CMPO/[C₂mim][NTf₂]的辐解及其对Eu³⁺萃取的影响

γ-Ray-Induced Radiolysis of CMPO/[C₂mim][NTf₂] and Its Effect on Eu³⁺ Extraction

RichHTML

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

推荐阅读 0