Complexation of UVI with 1-hydroxyethane-1,1-diphosphonic acid in acidic to basic solutions

被引:25
作者
Reed, Wendy A.
Rao, Linfeng [1 ]
Zanonato, PierLuigi
Garnov, Alexander Yu.
Powell, Brian A.
Nash, Kenneth L.
机构
[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Berkeley, CA 94720 USA
[2] Washington State Univ, Dept Chem, Pullman, WA 99164 USA
关键词
D O I
10.1021/ic0621401
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Complexation of U-VI with 1-hydroxyethane-1,1-diphosphonic acid (HEDPA) in acidic to basic solutions has been studied with multiple techniques. A number of 1:1 (UO2H3L), 1:2 (UO2HjL2 where j = +4, +3, +2, +1, 0, and -1), and 2:2 [(UO2)(2)HjL2 where j = +1, 0, and -1] complexes form, but the 1:2 complexes are the major species in a wide pH range. Thermodynamic parameters (formation constants and enthalpy and entropy of complexation) were determined by potentiometry and calorimetry. Data indicate that the complexation of U-VI with HEDPA is exothermic, favored by the enthalpy of complexation. This is in contrast to the complexation of U-VI with dicarboxylic acids in which the enthalpy term usually is unfavorable. Results from electrospray ionization mass spectrometry and P-31 NMR have confirmed the presence of 1:1, 1:2, and 2:2 U(VI)HEDPA complexes.
引用
收藏
页码:2870 / 2876
页数:7
相关论文
共 29 条
[1]  
ARNEK R, 1970, ARK KEMI, V32, P81
[2]   COMPLEXATION OF THE URANYL-ION WITH THE AMINOMETHYLENEDIPHOSPHONATES MAMDP AND AMDP [J].
BOLLINGER, JE ;
ROUNDHILL, DM .
INORGANIC CHEMISTRY, 1994, 33 (26) :6421-6424
[3]  
BOND AH, 2000, MAT RES SOC S P SCI, V608, P595
[4]  
BUDAVARI S, 1989, MERCK INDEX, P606
[5]   ON ACIDITY OF SUBSTITUTED METHYLENEDIPHOSPHONATES AND THEIR INTERACTION WITH ALKALI METAL IONS [J].
CARROLL, RL ;
IRANI, RR .
INORGANIC CHEMISTRY, 1967, 6 (11) :1994-&
[6]   DETERMINATION OF FORMATION-CONSTANTS OF CALCIUM COMPLEXES OF DIFLUOROMETHYLENEDIPHOSPHONIC ACID AND RELATED DIPHOSPHONATES [J].
FONONG, T ;
BURTON, DJ ;
PIETRZYK, DJ .
ANALYTICAL CHEMISTRY, 1983, 55 (07) :1089-1094
[7]   Investigation of equilibria in solution. Determination of equilibrium constants with the HYPERQUAD suite of programs [J].
Gans, P ;
Sabatini, A ;
Vacca, A .
TALANTA, 1996, 43 (10) :1739-1753
[8]   Leaching of U(VI), Am(III), and Sr(II) from simulated tank waste sludges [J].
Garnov, AY ;
Rao, LF ;
Nash, KL ;
Bond, AH .
SEPARATION SCIENCE AND TECHNOLOGY, 2003, 38 (02) :359-374
[9]   DETERMINATION OF THE EQUIVALENCE POINT IN POTENTIOMETRIC TITRATIONS .2. [J].
GRAN, G .
ANALYST, 1952, 77 (920) :661-671
[10]   Permafrost monitoring in the high mountains of Europe:: the PACE project in its global context [J].
Harris, C ;
Haeberli, W ;
Vonder Mühll, D ;
King, L .
PERMAFROST AND PERIGLACIAL PROCESSES, 2001, 12 (01) :3-11