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JNCTJ8410 2004-006 2004 3 ( ) UPRISE Nd 250mL 0.2 mol Nd Nd (FP)DF DOBA DOiBA NN'-2--1.6 mol/l NN'- -1.7 mol/l NN'-1.5 mol/l DOBA 1mol/L 3.5mol/L 2 NN'--1.7 mol/l NN' -1.5 mol/l ZrRu Ce DF 150 100 Sr Mo Pd DF Nd 1 NN'-2--1.6 mol/l DF FP 100 Nd Pd DF 100 1 2 --
March, 2004 The dissolving test of the uranium oxide using amide system extraction solvent (Document Prepared by Other Organization, Based on the Contract) Mizuno Mineo 1 Kosaka Yuji 1 Mori Yukihide 2 Shimada Takashi 2 Abstract The process ( the UPRISE method ) of dissolving uranium and plutonium selectively and separating from oxide fuel using the amide system extraction solvent have been investigated. By the cold test which used Nd oxide so far, the dissolving of Nd with about 0.2 mol to the solvent of 250mL is confirmed. In this work, the investigations of the dissolving tendency of uranium to the amide system extraction solvent and decontamination factor(df) of the typical fission product (FP) such as Nd were carried out, and following results are obtained. In the test of the same dissolving conditions, the uranium dissolving rate to extraction solvent DOBA was approximately equivalent to the case of the DOiBA. Three kinds of extraction solvent were examined in the same dissolving condition, the difference of the uranium dissolving rate was observed. The results of the dissolving rates indicated the order of NN'-hexyl-2,ethyl-hexan-amid-1.6 mol/l nitric acid complex >NN'-dibutyl-butyl-amid-1.7 mol/l nitric acid complex >NN'-di-isobutyl-isobutyl-amid- 1.5 mol/l nitric acid complex. In the case of DOBA extraction solvent, the dissolving rate increased by about 2 order with the increase of the nitric acid concentration from 1mol/L up to 3.5mol/L and strong influence of the nitric acid concentration was confirmed to the dissolving rate. In the tests with the NN'-dibutyl-butyl-amid-1.7 mol/l nitric acid complex and NN'-di-isobutyl-isobutyl-amid-1.5 mol/l nitric acid complex, the DF values of Zr, Ru and Ce increased with the elapse of the test duration and exceeded 100 after 150 hours of test duration. On the other hand, the DF value indicated around 1 for Sr, Mo and Pd, and around 0.1 for Nd. In the test with the NN'-hexyl-2-ethyl-hexan-amid-1.6 mol/l nitric acid complex, significant difference wasn't observed in the tendency of the elapsed change among the DF values of the FP elements. The DF values of all FP elements except Nd and Pd exceeded 100 after 100 hours of test duration. This work was performed by Mitsubishi Heavy Industries Ltd. under contract with Japan Nuclear Cycle Development Institute. JNC Liaison:Recycle Process Technology Group, Advanced Fuel Recycle Technology Division, Waste Management and Fuel Cycle Research Center, Tokai Works JNC 1 Nuclear development Inc. 2 Mitsubishi Heavy Industries, Ltd. --
JNCTJ8410 2004-006 1 1 43 4.1 4.2 4.3 4.4 65 56 65 67 67 5.1 5.2 9 9 9 64 32 6.1 364 2 6.2 FP 365 2 71 42 72 73 --
2.1 ----------------------------------------- 2 2.2 J11J14 ----------------------------------------------- 3 4.1 5.1 5.2 5.3 5.4 5.5 5.6 5.7 5.8 5.9 ------------------------------------ 8 -------------------------- 14 (1) ------------------------ 15 (2) ------------------------ 16 (3) ------------------------ 17 (4) ------------------------ 18 DOBA-1mol/L J8 ------------------------- 19 DOBA-3.5mol/L J9 ----------------------- 20 DOiBA-3.4mol/L J10 ---------------------- 21 DOBA-3.5mol/L FP J11 ----- 22 5.10 NN'--1.7mol/L FP J12 -------------------------------------------------------------------------- 5.11 NN'-1.5mol/L FP J13 ------------------------------------------------------------------ 5.12 NN'-2--1.6mol/L FP J11 ------------------------------------------------------------------ 5.13 J11 DF --------------------------------------------------- 5.14 J11 DF 2 -------------------------------------------------- 5.15 J11 DF 3 -------------------------------------------------- 5.16 J12 DF -------------------------------------------------- 5.17 J12 DF 2 -------------------------------------------------- 5.18 J13 DF -------------------------------------------------- 5.10 J13 DF 2 -------------------------------------------------- 5.20 J14 DF -------------------------------------------------- 5.21 J14 DF 2 -------------------------------------------------- 23 24 25 26 27 28 29 30 31 32 33 34 --
3.1 ------------------------------------ 5 5.1 -------------------------------------------------- 35 5.2 DOBA-1mol/L J8 -------------- 36 5.3 DOBA-3.5mol/L J9 U ---------- 37 5.4 DOiBA-3.4mol/L J10 U -------- 38 5.5 DOBA-3.5mol/L FP J11 U ------------------------------------------------------------------------------ 5.6 DOBA-3.5mol/L FP J11 DF ---- 40 5.7 NN'--1.7mol/L FP J12 U --------------------------------------------------------------- 5.8 NN'--1.7mol/L FP J12 DF ----------------------------------------------------------------------------- 5.9 NN'-1.5mol/L FP J13 U --------------------------------------------------------------- 5.10 NN'-1.5mol/L FP J13 DF ----------------------------------------------------------------------------- 5.11 NN'-2--1.6mol/L FP J14 U ------------------------------------------------------------ 45 5.12 NN'-2--1.6mol/L FP J14 DF ----------------------------------------------------------------------------- 6.1 U J9, J10 ------------------ 66 6.2 U J9, J10 --------- 67 6.3 U J12,J13,J14 ------------ 68 6.4 U J8, J9 --------------------- 69 6.5 DOBA-3.5mol/L FP FP DF --------------------------------------------------------------------------- 39 41 42 43 44 46 70 --
5.1 DOBA-1mol/L J8 1---------------------------- 47 5.2 DOBA-1mol/L J8 2---------------------------- 48 5.3 DOBA-3.5mol/L J9 1-------------------------- 49 5.4 DOBA-3.5mol/L J9 2-------------------------- 50 5.5 DOiBA-3.4mol/L J10 1------------------------- 51 5.6 DOiBA-3.4mol/L J10 2------------------------- 52 5.7 DOBA-3.5mol/L, FP J11 1------ 53 5.8 DOBA-3.5mol/L, FP J11 2------- 54 5.9 NN'--1.7mol/L FP J12 1-------------------------------------------------------------------- 5.10 NN'--1.7mol/L FP J12 2--------------------------------------------------------------------- 5.11 NN'--1.7mol/L FP J12 ------------------------------------------ 57 5.12 NN'--1.5mol/L FP J13 1-------------------------------------------------------------------- 5.13 NN'--1.5mol/L FP J13 2--------------------------------------------------------------------- 5.14 NN'--1.5mol/L FP J13 ------------------------------------------- 60 5.15 NN'--2--1.6mol/L FP J14 1-------------------------------------------------------------------- 5.16 NN'--2--1.6mol/L FP J14 2--------------------------------------------------------------------- 5.17 NN'--2--1.6mol/L FP J14 ----------------------------------------------- 63 55 56 58 59 61 62 --
UPRISE Nd 250mL 0.2 mol Nd Nd (FP) (1) 2.1 H13 1) 17gU 1) UO 2 UO 2 90m 75106m 60g J8J10 2) FP UO 2 1) 90m 75106m 80g FP 2.2 FP FP J11J14 (2) 2.1 1mol/L 3.5mol/L 1 200mL - 1 -
2.1 J8 DOBA- 1 mol/l H14 J9 J10 DOBA- 3.5 mol/l DOiBA- 3.4 mol/l UO 2 90m J11 DOBA- 3.5 mol/l 40 H15 J12 J13 NN'- -1.7 mol/l NN' -1.5 mol/l UO 2 90mNd 2 O 3, ZrO 2, SrO, Pd, MoO 3, RuO 2,CeO 2 J14 NN'-2- -1.6 mol/l - 2 -
2.2 J11J14 U FP UO2 SrO ZrO2 MoO3 RuO2 Pd CeO2 Nd2O3 (g) 19.24 0.088 0.18 0.25 0.21 0.18 0.30 0.47 20.93 wt% 91.95 0.42 0.88 1.19 1.02 0.88 1.43 2.24 100.00 90m( ) 12 18 m*1 5.3 m*2 200mesh *2 10 20 m*2 82 m*2 82 m*2 2N 3N 3N 3N 3N 3N 3N *1 *2-3 -
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2.1 15 45 FP Nd 4.1 2mL ICP 1 2 2mL 30120 5 4.1 4.2 200mL 1 2mL - 6 -
2 2mL 2mL 45 4.3 FP TBP ICP FP FP ICP 1mol/L-NaOH 4.4 (1) J8J14 (2) FP FP (DF ) DF(FP/U)SA(FP/U)LA (4.1) (FP/U)SA FP/U (FP/U)LA FP/U FP DF - 7 -
4.1 J8 DOBA-1mol/L H14 H15 J9 J10 J11 J12 J13 J14 DOBA-3.5mol/L DOiBA-3.4mol/L DOBA-3.5mol/L NN'- -1.7 mol/l NN' -1.5 mol/l NN'-2- -1.6mol/L UO 2 90m UO2 90m FPNd2O3, ZrO2, SrO, Pd, MoO3, RuO2, CeO2) 17gUUO 2 19.24g 17gUUO2 19.24g FP7 1.7g 200mL 405 1030 45 2mL - 8 -
5.1 2.1 5.1 5.1 20 J10 J8 1mol/L J8 3.4mol/L Nd (FP) J11 DOBA-1mol/L DOBA-3.5mol/L J12J14 NN'-NN' NN'-2-3 JNC Nd 1.5 mol/l 5.2 J8J14 5.2 5.5 5.6 5.12 5.1 5.17 5.2 5.5 (1) DOBA-1mol/L J8-9 -
2 40 22 1 30 90 292 10 1:10 2 1 5.2 J8 292 2.4% (2) DOBA-3.5mol/L J9 2 3540 4 40 79 5.3 J9 139 (3) DOiBA-3.4mol/L J10 4 10 1 40-10 -
19 5 30 79 5.4 J10 79 (4) DOBA-3.5mol/L FP J11 4 J10 FP 40 9 1 40 5 60 132 5.5 J11 132 98.1% 2.24mol/L J9 2.32 (4.1) J11 FP DF 5.6 FP DF 5.13 5.15 (5) NN'--1.7 mol/l FP J12 1.7 mol/l FP 2 40 23 1 60 90 323 5.11 FP 5.11-11 -
5.7 J12 323 9.9% 0.1mol/L J12 FP DF 5.8 FP DF 5.16 5.17 (6) NN'-1.5 mol/l FP J13 2 40 18 1 60 90 318 5.9 J13 318 5.3% J12 9.9% 5.14 J12 5.14 121.7% 5.4 150mL J12 22 ml J13 FP DF 5.10 FP DF 5.18 5.19 (7) NN'-2--1.6 mol/l FP J14 5 4023 1 J12 J13 2 FP 60 90 317-12 -
5.17 2 J12 J13 5.17 5.11 J14 323 30.9% 0.3mol/L J14 J12 J13 J14 FP DF 5.12 FP DF 5.20 5.21-13 -
5.1 (mol/l) DOBA- 1 mol/l 0.992 J8 DOiBA- 3.4 mol/l 3.442 J10 DOBA- 3.5 mol/l 3.508 J9, J11 NN'- -1.7 mol/l 1.683 J12 NN' -1.5 mol/l 1.500 J13 NN'-2- -1.6mol/L 1.592 J14-14 -
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0 23 83 5.9 NN'--1.7 mol/l FP J12(1) - 55 -
143 233 323 5.10 NN'--1.7 mol/l FP J12(2) - 56 -
5.11 NN'--1.7 mol/l FP J12-57 -
0 18 138 5.12 NN'-1.5 mol/l FP J13(1) - 58 -
138 228 78 5.13 NN'-1.5 mol/l FP J13(2) - 59 -
5.14 NN'-1.5 mol/l FP J13-60 -
17 77 5.15 N'-2--1.6 mol/l FP J14(1) - 61 -
137 227 317 5.16 N'-2--1.6 mol/l FP J14(2) - 62 -
5.17 NN'-2--1.6 mol/l FP J14-63 -
6.1 (1) 2 DOBA DOiBA J9 J10 6.1 6.2 6.1 DOBA(J9) DOiBA(J10) 40 DOiBA(J10) DOBA(J9) 2.45.9 6.2 40 DOiBA(J10) DOBA(J9) 0.140.18mol/L DOiBA(J10) DOBA(J9) DOiBA DOBA DOiBA DOBA FP 1.51.7 mol/l 3 NN'--1.7 mol/l NN' -1.5 mol/l NN'-2--1.6 mol/l J12J14 6.3 6.3 J14 30% J12 J13 NN'-2- (2) DOBA 1mol/L 3.5mol/L J8J9 6.4 6.4 1mol/L J8 293 2.4% 3.5mol/L J9 139 40 J8J9 20 J8 139 1% 1mol/L 3.5mol/L 2-64 -
6.2 FP DOBA-3.5mol/L J11 Ru Ce 2 2 (4.1) FP/U 5.6 DF DF Sr Zr 2 42 132 0.001mg/mL Ru Ce DF MoPd Nd 3 40 12 132 DF Mo DF 100 Pd Nd 2 DF 10100 6.5 J11 DF 5.6 DF 5.5 NN'--1.7 mol/l J12 5.8 ZrRu Ce DF 150 100 SrMo Pd DF Nd 1 NN'-1.5 mol/l J13 5.10 Mo DF J12 Ce J12 ZrRu CeDF100Sr Mo PdDFNdDF DF FP NN'-2--1.6 mol/l J14 5.12 FP DF J14 100 Nd Pd DF 100 J12 J13 J12 J13 NN'--1.7 mol/l NN' -1.5 mol/l SrMoPd Nd NN'-2--1.6 mol/l - 65 -
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UO 2 DOBA DOiBA UO 2 NN'-2--1.6 mol/l NN'- -1.7 mol/l NN'-1.5 mol/l DOBA 1mol/L 3.4mol/L 2 NN'--1.7 mol/l NN' -1.5 mol/l ZrRu Ce DF 150 100 SrMo Pd DF Nd 1 NN'--1.7 mol/l NN' -1.5 mol/l SrMoPd Nd NN'-2--1.6 mol/l NN'-2--1.6 mol/l DF FP 100 Nd Pd DF 100-71 -
TBP TBP DF TBP TBP NOX scf-co 2 scf-co 2-72 -
1) TBP JNC TJ8400 2003-013 (2002) - 73 -