In-Situ-Generated Fluoride-Assisted Rapid Dissolution of Uranium Oxides by Ionic Liquids

被引:6
作者
Goyal, Priya [1 ]
Sengupta, Arijit [1 ,4 ]
Srivastava, Ashutosh [1 ]
Mukherjee, Sumanta [2 ]
Rout, Vaibhavi V. [3 ]
Mohapatra, Prasanta K. [1 ,4 ]
机构
[1] Bhabha Atom Res Ctr, Radiochem Div, Mumbai 400085, India
[2] Bhabha Atom Res Ctr, Prod Dev Div, Mumbai 400085, India
[3] Bhabha Atom Res Ctr, Radioanalyt Chem Div, Mumbai 400085, India
[4] Homi Bhabha Natl Inst, Mumbai 400094, India
关键词
ELECTROCHEMICAL-BEHAVIOR; DIRECT ELECTRODEPOSITION; EXTRACTION; URANYL; SPECIATION; KINETICS; COMPLEXATION; ADSORPTION; STABILITY; MECHANISM;
D O I
10.1021/acs.inorgchem.3c04075
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
A quantitative, rapid, endothermic dissolution of U3O8 in C(4)mim<middle dot>PF6 (1-alkyl-3-methyl imidazolium hexafluorophosphate) has been achieved within 2 h at 65 degrees C by in situ generated fluoride ions by pre-equilibrating the ionic liquid with suitable concentrations of nitric acid. The efficiency of the dissolution followed the trend: UO3 > UO2 > U3O8. The fluoride generation was found to increase with the concentration of nitric acid being equilibrated, the water content of the ionic liquid, and also the time of equilibration. The rate of dissolution of U3O8 followed the trend: C(4)mim<middle dot>PF6> C(6)mim<middle dot>PF6 > C(8)mim<middle dot>PF6. The maximum loading observed for the present case was 200 mg mL(-1) which is considered to be quite high with an ionic liquid. The effects of different acid pre-equilibration (HClO4, HCl) on F- generation and subsequent dissolution characteristics have also been investigated. The in situ F- generation, as well as U(3)O8 dissolution, were found to predominantly follow a pseudo-second-order rate kinetics, while the rate constants for U3O8 dissolution were found to be higher than that of F- generation. The dissolved uranium was successfully electrodeposited on a Cu plate, as confirmed by EDXRF, while the formation of UO2 was revealed from the XRD pattern of the deposit.
引用
收藏
页码:7161 / 7176
页数:16
相关论文
共 66 条
[11]   Novel Poly(ionic liquid) Augmented Membranes for Unconventional Aqueous Phase Applications in Fractionation of Dyes and Sugar [J].
DePaz, Sandrina ;
Sengupta, Arijit ;
Chiao, Yu-Hsuan ;
Wickramasinghe, Sumith Ranil .
POLYMERS, 2021, 13 (14)
[12]  
Dieke G.H., 1949, SPECTROSCOPIC PROPER
[13]   Influence of solvent structural variations on the mechanism of facilitated ion transfer into room-temperature ionic liquids [J].
Dietz, ML ;
Dzielawa, JA ;
Laszak, I ;
Young, BA ;
Jensen, MP .
GREEN CHEMISTRY, 2003, 5 (06) :682-685
[14]   Ecofriendly fast synthesis of hydrophilic poly(ethyleneglycol)-ionic liquid matrices for liquid-phase organic synthesis [J].
Fraga-Dubreuil, J ;
Famelart, MH ;
Bazureau, JP .
ORGANIC PROCESS RESEARCH & DEVELOPMENT, 2002, 6 (04) :374-378
[15]   Direct Electrodeposition of UO2 from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System [J].
Freiderich, John W. ;
Wanigasekara, Eranda ;
Sun, Xiao-Guang ;
Meisner, Roberta A. ;
Meyer, Harry M., III ;
Luo, Huimin ;
Delmau, Laetitia H. ;
Dai, Sheng ;
Moyer, Bruce A. .
ELECTROCHIMICA ACTA, 2014, 115 :630-638
[16]   Uranyl coordination in ionic liquids:: The competition between ionic liquid anions, uranyl counterions, and Cl- anions investigated by extended X-ray absorption fine structure and UV-visible spectroscopies and molecular dynamics simulations [J].
Gaillard, C. ;
Chaumont, A. ;
Billard, I. ;
Hennig, C. ;
Ouadi, A. ;
Wipff, G. .
INORGANIC CHEMISTRY, 2007, 46 (12) :4815-4826
[17]   Competitive Complexation of Nitrates and Chlorides to Uranyl in a Room Temperature Ionic Liquid [J].
Gaillard, C. ;
Chaumont, A. ;
Billard, I. ;
Hennig, C. ;
Ouadi, A. ;
Georg, S. ;
Wipff, G. .
INORGANIC CHEMISTRY, 2010, 49 (14) :6484-6494
[18]   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
[19]   COUPLING SCHEME IN URANYL COMPLEXES [J].
GORLLERW.C ;
VANQUICK.LG .
JOURNAL OF CHEMICAL PHYSICS, 1972, 57 (04) :1436-&
[20]   IDENTIFICATION OF LOWER TRANSITIONS IN SPECTRA OF URANYL COMPLEXES [J].
GORLLERW.C ;
VANQUICKENBORNE, LG .
JOURNAL OF CHEMICAL PHYSICS, 1971, 54 (10) :4178-+