CMPO和TBP在离子液体中选择性萃取水溶液中铀酰离子的研究

doi:10.3866/PKU.WHXB2014Ac10

摘要/Abstract

摘要：

研究了以辛基(苯基)-N,N-二异丁基胺甲酰基甲基氧化膦(CMPO)和磷酸三丁酯(TBP)在离子液体(ILs)中选择性萃取水溶液中的铀酰离子(UO₂²⁺). 离子液体为1-烷基-3-甲基咪唑双三氟甲基磺酰亚胺盐(C_nmimNTf₂,n=2, 4, 6, 8). 水相硝酸浓度以及离子液体的取代基链长对UO₂²⁺的分配比和萃取选择性均有影响. 与TBP相比, CMPO在离子液体中对UO₂²⁺具有更高的萃取分配比和更好的萃取选择性. 对模拟废液(SLW)萃取发现,Zr⁴⁺, ReO₄^- 和Cs⁺是主要的竞争离子. ReO₄^-和Cs⁺可被离子液体本身萃取, 而Zr⁴⁺则是被CMPO和TBP萃取而不被离子液体本身萃取. 本研究工作表明, CMPO-ILs 体系在铀酰离子的选择性萃取分离中具有一定的应用前景.

关键词: 离子液体, 萃取, 分离, 选择性, 铀酰离子

Abstract:

The selective extraction of UO₂²⁺ from aqueous solution in the presence of other metal ions by octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) and tri-n-butyl phosphate (TBP) in ionic liquids (ILs), namely 1-alkyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imides (C_nmimNTf₂, n=2, 4, 6, 8), were studied. The influences of the nitric acid concentration and the IL alkyl chain length on the distribution ratio and selectivity were examined. Compared with TBP in C4mimNTf2, CMPO in the ILs gave higher distribution ratios and better selectivities. Zr⁴⁺, ReO₄^-, and Cs⁺ were the main competing ions in the separation of UO₂²⁺ from simulated liquid waste (SLM) by the C_nmimNTf₂ systems. ReO₄^- and Cs⁺ were extracted by the ILs themselves. Zr⁴⁺ was extracted by CMPO or TBP in the ILs but not by the ILs themselves. This work gives further information on the use of ILs, and provides a basis for matching extractants with ILs in the processing of spent nuclear fuel.

Key words: Ionic liquid, Extraction, Separation, Selectivity, UO₂²⁺

孙涛祥, 沈兴海, 陈庆德. CMPO和TBP在离子液体中选择性萃取水溶液中铀酰离子的研究[J]. 物理化学学报, 2015, 31(Suppl), 32-38. doi: 10.3866/PKU.WHXB2014Ac10

SUN Tao-Xiang, SHEN Xing-Hai, CHEN Qing-De. Investigation of Selective Extraction of UO₂²⁺ from Aqueous Solution by CMPO and TBP in Ionic Liquids[J]. Acta Phys. -Chim. Sin. 2015, 31(Suppl), 32-38. doi: 10.3866/PKU.WHXB2014Ac10

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB2014Ac10

https://www.whxb.pku.edu.cn/CN/Y2015/V31/ISuppl/32

参考文献

(1) Hallett, J. P.; Welton, T. Chem. Rev. 2011, 111, 3508. doi: 10.1021/cr1003248
(2) Zhao, D. B.; Wu, M.; Kou, Y.; Min, E. Z. Catal. Today 2002, 74, 157. doi: 10.1016/S0920-5861(01)00541-7
(3) Armand, M.; Endres, F.; MacFarlane, D. R.; Ohno, H.; Scrosati, B. Nat. Mater. 2009, 8, 621. doi: 10.1038/nmat2448
(4) Huddleston, J. G.; Willauer, H. D.; Swatloski, R. P.; Visser, A. E.; Rogers, R. D. Chem. Commun. 1998, 1765.
(5) Sun, X. Q.; Luo, H. M.; Dai, S. Chem. Rev. 2012, 112, 2100. doi: 10.1021/cr200193x
(6) Dai, S.; Ju, Y. H.; Barnes, C. E. J. Chem. Soc. Dalton Trans. 1999, 28, 1201.
(7) Visser, A. E.; Swatloski, R. P.; Reichert, W. M.; Griffin, S. T.; Rogers, R. D. Ind. Eng. Chem. Res. 2000, 39, 3596. doi: 10.1021/ie000426m
(8) Dietz, M. L.; Dzielawa, J. A. Chem. Commun. 2001, 2124.
(9) Jensen, M. P.; Dzielawa, J. A.; Rickert, P.; Dietz, M. L. J. Am. Chem. Soc. 2002, 124, 10664. doi: 10.1021/ja027476y
(10) Jensen, M. P.; Neuefeind, J.; Beitz, J. V.; Skanthakumar, S.; Soderholm, L. J. Am. Chem. Soc. 2003, 125, 15466. doi: 10.1021/ja037577b
(11) Luo, H. M.; Dai, S.; Bonnesen, P. V. Anal. Chem. 2004, 76, 2773. doi: 10.1021/ac035473d
(12) Luo, H. M.; Dai, S.; Bonnesen, P. V.; Buchanan, A. C.; Holbrey, J. D.; Bridges, N. J.; Rogers, R. D. Anal. Chem. 2004, 76, 3078. doi: 10.1021/ac049949k
(13) Dietz, M. L.; Stepinski, D. C. Green Chem. 2005, 7, 747. doi: 10.1039/b508604c
(14) Ouadi, A.; Klimchuk, O.; Gaillard, C.; Billard, I. Green Chem. 2007, 9, 1160. doi: 10.1039/b703642f
(15) Giridhar, P.; Venkatesan, K. A.; Srinivasan, T. G.; Rao, P. R. V. J. Radioanal. Nucl. Chem. 2005, 265, 31.
(16) Giridhar, P.; Venkatesan, K. A.; Subramaniam, S.; Srinivasan, T. G.; Rao, P. R. V. J. Alloy. Compd. 2008, 448, 104. doi: 10.1016/j.jallcom.2007.03.115
(17) Rao, P. R. V.; Venkatesan, K. A.; Srinivasan, T. G. Prog. Nucl. Energy 2008, 50, 449. doi: 10.1016/j.pnucene.2007.11.079
(18) Dietz, M. L.; Stepinski, D. C. Talanta 2008, 75, 598. doi: 10.1016/j.talanta.2007.11.051
(19) Billard, I.; Ouadi, A.; Jobin, E.; Champion, J.; Gaillard, C.; Georg, S. Solvent Extr. Ion Exch. 2011, 29, 577. doi: 10.1080/07366299.2011.566494
(20) Bell, T. J.; Ikeda, Y. Dalton Trans. 2011, 40, 10125. doi: 10.1039/c1dt10755k
(21) Sun, T. X.; Shen, X. H.; Chen, Q. D.; Ma, J. Y.; Zhang, S.; Huang, Y. Y. Radiat. Phys. Chem. 2013, 83, 74. doi: 10.1016/j.radphyschem.2012.10.004
(22) Srncik, M.; Kogelnig, D.; Stojanovic, A.; Korner, W.; Krachler, R.; Wallner, G. Appl. Radiat. Isotopes 2009, 67, 2146. doi: 10.1016/j.apradiso.2009.04.011
(23) Wang, J. S.; Sheaff, C. N.; Yoon, B.; Addleman, R. S.; Wai, C. M. Chem. -Eur. J. 2009, 15, 4458. doi: 10.1002/chem.v15:17
(24) Stepinski, D. C.; Vandegrift, G. F.; Shkrob, I. A.; Wishart, J. F.; Kerr, K.; Dietz, M. L.; Qadah, D. T. D.; Garvey, S. L. Ind. Eng. Chem. Res. 2010, 49, 5863. doi: 10.1021/ie1000345
(25) Xu, C.; Yuan, L. Y.; Shen, X. H.; Zhai, M. L. Dalton Trans. 2010, 39, 3897. doi: 10.1039/b925594j
(26) Xu, C.; Shen, X. H.; Chen, Q. D.; Gao, H. C. Sci. China Ser. B 2009, 52, 1858.
(27) Sun, X. Q.; Bell, J. R.; Luo, H. M.; Dai, S. Dalton Trans. 2011, 40, 8019. doi: 10.1039/c1dt10873e
(28) Bonnaffe-Moity, M.; Ouadi, A.; Mazan, V.; Miroshnichenko, S.; Ternova, D.; Georg, S.; Sypula, M.; Gaillard, C.; Billard, I. Dalton Trans. 2012, 41, 7526. doi: 10.1039/c2dt12421a
(29) Rout, A.; Karmakar, S.; Venkatesan, K. A.; Srinivasan, T. G.; Rao, P. R. V. Sep. Purif. Technol. 2011, 81, 109. doi: 10.1016/j.seppur.2011.04.033
(30) Hawkins, C. A.; Garvey, S. L.; Dietz, M. L. Sep. Purif. Technol. 2012, 89, 31. doi: 10.1016/j.seppur.2011.12.004
(31) Harmon, C. D.; Smith, W. H.; Costa, D. A. Radiat. Phys. Chem. 2001, 60, 157. doi: 10.1016/S0969-806X(00)00336-4
(32) Visser, A. E.; Jensen, M. P.; Laszak, I.; Nash, K. L.; Choppin, G. R.; Rogers, R. D. Inorg. Chem. 2003, 42, 2197. doi: 10.1021/ic026302e
(33) Cocalia, V. A.; Jensen, M. P.; Holbrey, J. D.; Spear, S. K.; Stepinski, D. C.; Rogers, R. D. Dalton Trans. 2005, 1966.
(34) Shen, Y. L.; Tan, X.W.; Wang, L.; Wu, W. S. Sep. Purif. Technol. 2011, 78, 298. doi: 10.1016/j.seppur.2011.01.042
(35) Rout, A.; Venkatesan, K. A.; Srinivasan, T. G.; Rao, P. R. V. J. Hazard. Mater. 2012, 221, 62.
(36) Bonhote, P.; Dias, A. P.; Papageorgiou, N.; Kalyanasundaram, K.; Grätzel, M. Inorg. Chem. 1996, 35, 1168. doi: 10.1021/ic951325x
(37) Ansari, S. A.; Prabhu, D. R.; Gujar, R. B.; Kanekar, A. S.; Rajeswari, B.; Kulkarni, M. J.; Murali, M. S.; Babu, Y.; Natarajan, V.; Rajeswari, S.; Suresh, A.; Manivannan, R.; Antony, M. P.; Srinivasan, T. G.; Manchanda, V. K. Sep. Purif. Technol. 2009, 66, 118. doi: 10.1016/j.seppur.2008.11.019
(38) Choppin, G.; Liljenzin, J. O.; Rydberg, J. Radiochemistry and Nuclear Chemistry, 3rd ed.; Elsevier Books: Oxford, 2002.
(39) Dietz, M. L.; Dzielawa, J. A.; Laszak, I.; Young, B. A.; Jensen, M. P. Green Chem. 2003, 5, 682. doi: 10.1039/b310507p
(40) Sun, T. X.; Wang, Z. M.; Shen, X. H. Inorg. Chim. Acta 2012, 390, 8. doi: 10.1016/j.ica.2012.04.005
(41) Lieser, K. H.; Kruger, A.; Singh, R. N. Radiochim. Acta 1981, 28, 97.
(42) Chaumont, A.; Klimchuk, O.; Gaillard, C.; Billard, I.; Ouadi, A.; Hennig, C.; Wipff, G. J. Phys. Chem. B 2012, 116, 3205. doi: 10.1021/jp209476h
(43) Rout, A.; Venkatesan, K. A.; Srinivasan, T. G.; Rao, P. R. V. Sep. Purif. Technol. 2011, 76, 238. doi: 10.1016/j.seppur.2010.10.009
(44) Fletcher, J. M.; Jenkins, I. L.; Lever, F. M.; Martin, F. S.; Powell, A. R.; Todd, R. J. Inorg. Nucl. Chem. 1955, 1, 378. doi: 10.1016/0022-1902(55)80048-6

[1]	曹玥晗, 郭瑞, 马敏智, 黄泽皑, 周莹. 活性位点电子密度变化对光催化CO₂活化和选择转化的影响[J]. 物理化学学报, 2024, 40(1): 2303029 - .
[2]	高凤雨, 刘恒恒, 姚小龙, Sani Zaharaddeen, 唐晓龙, 罗宁, 易红宏, 赵顺征, 于庆君, 周远松. 球形表面富锰Mn_xCo_3−xO_4−ƞ尖晶石型催化剂选择性催化还原NO_x研究[J]. 物理化学学报, 2023, 39(9): 2212003 -0 .
[3]	袁干印, 奚政, 王楚, 孙晓环, 韩杰, 郭荣. 超分子手性聚苯胺-金复合纳米酶的构建及其对映选择性催化[J]. 物理化学学报, 2023, 39(7): 2212061 -0 .
[4]	王中辽, 汪静, 张金锋, 代凯. 光激发电荷在光催化氧化还原反应中的全利用[J]. 物理化学学报, 2023, 39(6): 2209037 - .
[5]	董少明, 普颖慧, 牛一鸣, 张蕾, 王永钊, 张炳森. 间隙碳调控Ni实现1,3-丁二烯高效加氢[J]. 物理化学学报, 2023, 39(11): 2301012 - .
[6]	胡程, 黄洪伟. 压电极化增强光催化能源转化的研究进展[J]. 物理化学学报, 2023, 39(11): 2212048 - .
[7]	谢垚, 张启涛, 孙宏丽, 滕镇远, 苏陈良. 聚合物半导体光催化合成过氧化氢：光氧化还原中心的空间分离和协同利用[J]. 物理化学学报, 2023, 39(11): 2301001 - .
[8]	蔡晓燕, 杜家豪, 钟光明, 张一鸣, 毛梁, 娄在祝. S-型异质结CeO₂/Zn_xCd_1−xIn₂S₄空心结构的构建及其可见光分解水制氢性能[J]. 物理化学学报, 2023, 39(11): 2302017 - .
[9]	方洪燕, 江静静, 王定胜, 刘向文, 朱敦如, 李亚栋. 乙炔半加氢催化剂设计[J]. 物理化学学报, 2023, 39(10): 2305030 - .
[10]	王天杰, 王耀伟, 陈宇辉, 刘建鹏, 史会兵, 郭丽敏, 赵志伟, 刘春太, 彭章泉. 锂-空气电池的实用化之路：规避二氧化碳负面效应[J]. 物理化学学报, 2022, 38(8): 2009071 - .
[11]	崔柏桦, 施毅, 李根, 陈亚楠, 陈伟, 邓意达, 胡文彬. 海水电解面临的挑战与机遇：含氯电化学中先进材料研究进展[J]. 物理化学学报, 2022, 38(6): 2106010 - .
[12]	李少鹏, 杜靖, 张彬, 刘艳贞, 梅清清, 孟庆磊, 董明华, 杜鹃, 赵志娟, 郑黎荣, 韩布兴, 赵美廷, 刘会贞. 利用空间位阻和氢溢流协同作用促进5-羟甲基糠醛选择性加氢制备5-甲基糠醛[J]. 物理化学学报, 2022, 38(10): 2206019 - .
[13]	郝磊端, 孙振宇. 基于金属氧化物材料的二氧化碳电催化还原[J]. 物理化学学报, 2021, 37(7): 2009033 - .
[14]	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 - .
[15]	孟怡辰, 况思宇, 刘海, 范群, 马新宾, 张生. 面向CO₂电化学转化的铜基催化剂研究进展[J]. 物理化学学报, 2021, 37(5): 2006034 - .