The application of novel hydrophobic ionic liquids to the extraction of uranium(VI) from nitric acid medium and a determination of the uranyl complexes formed

被引:66
作者
Bell, Thomas James [1 ]
Ikeda, Yasuhisa [1 ]
机构
[1] Tokyo Inst Technol, Nucl Reactors Res Lab, Meguro Ku, Tokyo 1528550, Japan
基金
日本学术振兴会;
关键词
SUPERCRITICAL CARBON-DIOXIDE; ROOM-TEMPERATURE; AQUEOUS-SOLUTION; LANTHANIDES; METAL; MECHANISM; BEHAVIOR;
D O I
10.1039/c1dt10755k
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Novel ammonium based hydrophobic ionic liquids (ILs) have been synthesised and characterised, and their use in the liquid-liquid extraction of uranium(VI) from an aqueous nitric acid solution using tri-n-butyl phosphate (TBP), studied. On varying the nitric acid concentration, each IL was found to give markedly different results. Relatively hydrophilic ILs showed high uranium(VI) extractability at 0.01 M nitric acid solution which progressively decreased from 0.01 to 2 M HNO3 and then increased again as the nitric acid concentration was increased to 6 M. An analysis of the mechanisms involved for one such IL, pointed to cationic-exchange being the predominant route at low nitric acid concentrations whilst at high nitric acid concentrations, anionic-exchange predominated. Strongly hydrophobic ILs showed low extractability for nitric acid concentrations below 0.1 M but increasing extractability from 0.1 M to 6 M nitric acid. The predominant mechanism in this case involved the partitioning of a neutral uranyl complex. The uranyl complexes were found to be UO22+center dot(TBP)(3) for the cationic exchange mechanism, UO2(NO3)(2)(TBP)(2) for the neutral mechanism and UO2(NO3)(3)(-)center dot(TBP) for the anionic exchange mechanism.
引用
收藏
页码:10125 / 10130
页数:6
相关论文
共 25 条
[1]   An investigation of the radiochemical stability of ionic liquids [J].
Allen, D ;
Baston, G ;
Bradley, AE ;
Gorman, T ;
Haile, A ;
Hamblett, I ;
Hatter, JE ;
Healey, MJF ;
Hodgson, B ;
Lewin, R ;
Lovell, KV ;
Newton, B ;
Pitner, WR ;
Rooney, DW ;
Sanders, D ;
Seddon, KR ;
Sims, HE ;
Thied, RC .
GREEN CHEMISTRY, 2002, 4 (02) :152-158
[2]  
Archambeau S., 2009, International Patent App No, Patent No. [PCT/FR2009/050339, 2009050339]
[3]   Liquid-liquid extraction of actinides, lanthanides, and fission products by use of ionic liquids: from discovery to understanding [J].
Billard, Isabelle ;
Ouadi, Ali ;
Gaillard, Clotilde .
ANALYTICAL AND BIOANALYTICAL CHEMISTRY, 2011, 400 (06) :1555-1566
[4]   Lanthanides and actinides in ionic liquids [J].
Binnemans, Koen .
CHEMICAL REVIEWS, 2007, 107 (06) :2592-2614
[5]   Recent developments in the purex process for nuclear fuel reprocessing: Complexant based stripping for uranium/plutonium separation [J].
Birkett, JE ;
Carrott, MJ ;
Fox, OD ;
Jones, CJ ;
Maher, CJ ;
Roube, CV ;
Taylor, RJ ;
Woodhead, DA .
CHIMIA, 2005, 59 (12) :898-904
[6]   Identical extraction behavior and coordination of trivalent or hexavalent f-element cations using ionic liquid and molecular solvents [J].
Cocalia, VA ;
Jensen, MP ;
Holbrey, JD ;
Spear, SK ;
Stepinski, DC ;
Rogers, RD .
DALTON TRANSACTIONS, 2005, (11) :1966-1971
[7]   Anion concentration-dependent partitioning mechanism in the extraction of uranium into room-temperature ionic liquids [J].
Dietz, Mark L. ;
Stepinski, Dominique C. .
TALANTA, 2008, 75 (02) :598-603
[8]   Stereochemical effects on the mode of facilitated ion transfer into room-temperature ionic liquids [J].
Dietz, Mark L. ;
Jakab, Sandrine ;
Yamato, Kazuhiro ;
Bartsch, Richard A. .
GREEN CHEMISTRY, 2008, 10 (02) :174-176
[9]   Mutual Solubilities of water and hydrophobic ionic liquids [J].
Freire, Mara G. ;
Neves, Catarina M. S. S. ;
Carvalho, Pedro J. ;
Gardas, Ramesh L. ;
Fernandes, Ana M. ;
Marrucho, Isabel M. ;
Santos, Luis M. N. B. F. ;
Coutinho, Jooa A. P. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2007, 111 (45) :13082-13089
[10]   Extraction of uranium (VI) by 1.1 M tri-n-butylphosphate/ionic liquid and the feasibility of recovery by direct electrodeposition from organic phase [J].
Giridhar, P. ;
Venkatesan, K. A. ;
Subramaniam, S. ;
Srinivasan, T. G. ;
Rao, P. R. Vasudeva .
JOURNAL OF ALLOYS AND COMPOUNDS, 2008, 448 (1-2) :104-108