Extraction of actinide (III, IV, V, VI) ions and TcO4- byN,N,N',N'- tetraisobutyl-3-oxa-glutaramide

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The extraction behavior of U(VI), Np(V), Pu(IV), Am(III), and TcO{sub 4}{sup -} with N, N, N', N'-tetraisobutyl-3-oxa-glutaramide (TiBOGA) were investigated. An organic phase of 0.2 mol/L TiBOGA in 40/60% (V/V) 1-octanol/kerosene showed good extractability for actinides (III, IV, V VI) and TcO{sub 4}{sup -}from aqueous solutions of HNO{sub 3} (0.1 to 4 mol/L). At 25 C, the distribution ratio of the actinide ions (D{sub An}) generally increased as the concentration of HNO{sub 3} in the aqueous phase was increased from 0.1 to 4 mol/L, while the D{sub Tc} at first increased, then decreased, with a maximum of 3.0 at 2 ... continued below

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Tian, Guoxin; Zhang, Ping; Wang, Jianchen & Rao, Linfeng May 1, 2005.

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The extraction behavior of U(VI), Np(V), Pu(IV), Am(III), and TcO{sub 4}{sup -} with N, N, N', N'-tetraisobutyl-3-oxa-glutaramide (TiBOGA) were investigated. An organic phase of 0.2 mol/L TiBOGA in 40/60% (V/V) 1-octanol/kerosene showed good extractability for actinides (III, IV, V VI) and TcO{sub 4}{sup -}from aqueous solutions of HNO{sub 3} (0.1 to 4 mol/L). At 25 C, the distribution ratio of the actinide ions (D{sub An}) generally increased as the concentration of HNO{sub 3} in the aqueous phase was increased from 0.1 to 4 mol/L, while the D{sub Tc} at first increased, then decreased, with a maximum of 3.0 at 2 mol/L HNO{sub 3}. Based on the slope analysis of the dependence of D{sub M} (M = An or Tc) on the concentrations of reagents, the formula of extracted complexes were assumed to be UO{sub 2}L{sub 2}(NO{sub 3}){sub 2}, NpO{sub 2}L{sub 2}(NO{sub 3}), PuL(NO{sub 3}){sub 4}, AmL{sub 3}(NO{sub 3}){sub 3}, and HL{sub 2}(TcO{sub 4}) where L = TiBOGA. The enthalpy and entropy of the corresponding extraction reactions, {Delta}{sub r}H and {Delta}{sub r}S, were calculated from the dependence of D on temperature in the range of 15-55 C. For U(VI), Np(V), Am(III) and TcO{sub 4}{sup -}, the extraction reactions are enthalpy driven and disfavored by entropy ({Delta}{sub r}H < 0 and {Delta}{sub r}S < 0). In contrast, the extraction reaction of Pu(IV) is entropy driven and disfavored by enthalpy ({Delta}{sub r}H > 0 and {Delta}{sub r}S > 0). A test run with 0.2 mol/L TiBOGA in 40/60% 1-octanol/kerosene was performed to separate actinides and TcO{sub 4}{sup -} from a simulated acidic high-level liquid waste (HLLW), using tracer amounts of {sup 238}U(VI), {sup 237}Np(V), {sup 239}Pu(VI), {sup 241}Am(III) and {sup 99}TcO{sub 4}{sup -}. The distribution ratios of U(VI), Np(V), Pu(VI), Am(III) and TcO{sub 4}{sup -} were 12.4, 3.9, 87, > 1000 and 1.5, respectively, confirming that TiBOGA is a promising extractant for the separation of all actinides and TcO{sub 4}{sup -} from acidic HLLW. It is noteworthy that the extractability of TiBOGA for Np(V) from acidic HLLW (D{sub Np(V)} = 3.9) is much higher than that of many other extractants that have been studies for the separation of actinides from HLLW.

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  • Journal Name: Solvent Extraction and Ion Exchange; Journal Volume: 23; Journal Issue: 5; Related Information: Journal Publication Date: Sept./Oct.2005

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  • Report No.: LBNL--57031
  • Grant Number: DE-AC02-05CH11231
  • Office of Scientific & Technical Information Report Number: 862069
  • Archival Resource Key: ark:/67531/metadc792402

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  • May 1, 2005

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  • Dec. 19, 2015, 7:14 p.m.

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  • Dec. 16, 2016, 1:07 p.m.

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Tian, Guoxin; Zhang, Ping; Wang, Jianchen & Rao, Linfeng. Extraction of actinide (III, IV, V, VI) ions and TcO4- byN,N,N',N'- tetraisobutyl-3-oxa-glutaramide, article, May 1, 2005; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc792402/: accessed December 16, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.