HWAHAK KONGHAK Vol. 39, No. 1, February, 2001, pp. 36-42(Journal of the Korean Institute of Chemical Engineers)

TBP Re, Np U

(2000 6 22 , 2000 11 22 )

A Selective-Separation of Re, Np and Residual U from the Simulated Radwaste SolutionContaining the Oxidant of Np by Solvent Extraction with Tributyl Phosphate

Eil Hee Lee, Soo Ho Kim, Jae Gwan Lim, Kwang Wook Kim and Jae-Hyung Yoo

Korea Atomic Energy Research InstituteReceived 22 June 2000; accepted 22 November 2000)

Np 1 g/L NH4VO3 10 Re, Np U

TBP! " #$ %&'( )&' *+ ,- # ./.0 1234. Re, Np, U %&' .05 TBP

678 9:;4 O/A ?8 2 @7 9:;0"[1, 2],

? @ 6A B Am(Americium), Cm(Curium)C6 D

9E F GH IJ ALI(Annual Limit of Intake)KL

:M ICRP(International commission on radiation protection) 30

EN OPQ0" RS T 0" UV W6[3].

XY ZXE HLW9 Tc; TcO4 [, Tc(VII)" \] W^ ,

Np; IV$, V$ _ VI$" \] W0`, 2 M 9 a

" V$", 3 M 79 bcd(disproportionation) ,e EN IV

$ _ VI$ f\g6 hiV W6[4, 5]. gj U; NE kl

U(VI)" \] W6. mno" a" III$" \] W Am, Cm

p Yd$ 7q _ r 7 s T t

u" RS g6[1, 2]. &g vw9 x I U;

yX(fertile material)" 34z {"|

]}YVo" 34 1 u" RSg6.

,z Tc, Np; ~ 9" [, Tc O 8!

,e0" y8! 9, NpE O 8! ,eE y8

36

Re, Np U 37

r,

e

! 9 {"| 63 }o" 8! +

zQp y +zQ %8! 9 3

S 50" [1, 6] W kl PQ0" RS

g6.

Tc, NpE ~0" *Z~, 1~, ~, 2~

n $D ~ 3V W0#[1, 2, 4, 5], 9 TBP(tri-

butyl phosphate) Eg *Z P/6. TBP Eg TcE

; 0#, 'E U(uranium) & Zr(zirconium) 7q

9 Tc 76[7, 8]. gj NpE ; Np(VI) > Np(IV)

Np(V) 0", Np(V) ZO V(V), KMnO4, Ce(IV),

K2Cr2O7 E Yd# HAN(hydroxyl amine nitrate), U(IV), ferrous

sulfamate E 2 $ ; Np(VI)# Np(IV)"

d3 g6. mn# g Yd(KMnO4, K2Cr2O7, Ce(IV) )

E O Np kl Np(VI)" Yd3 70" kl T W

0#, f\ ' W, r Ru(Ruthenium)

; kl RuO4" Yd3 h V`, Ce(Cerium); TBP

; Ce(IV)" 1234 6[9, 10]. &g g Yd

70" Np(VI) Np(V)" 63 2 T 3 J

w S3 W6.

DD TBP Eg Tc, NpE F Cz UE :$

; ( 0.1 M 7)9 Tc, Np Up s 7 fV,

#D 7(raffinate) V \] W0" N

[, UE /: 734 9 a" $ V ,

) U 7Q0" ZO Q; ( 103M /:) \

] O9E ZO ''g / W6. r

W [, HLW" Tc, Np, UE PQ

f/ Kh vw9E 1g /6.

u9 9 1 [11, 12] p 0" Np

Np(VI)" Yd34, 'D V(V)

(NH4VO3) NpE Yd" P/ HLW" Tc, Np m '

\] W U PQ0" T W f/ Kh Q0"

6. m TcE " 1 [11] Tcp dQ

X ` TcE dQ $ CjQ0" *

V W Re(Rhenium :XYZX9 ReO4" \]) P/

6. ; OP NpE Yd$ $ 3 ReE '

0`, 60" 10) *(Np Yd" 1 g/L

NH4VO3 ) 70" Re, Np, UE fp E PQ

NF m % |1 3 V

6.

2.

2-1.

kE*; E v 7 B Re, Npp U, Yd$ III$

E MA(Minor Actinide) _ RE(Rare Earth elements)E i " Nd

(Neodymium) _ Y(Yttrium), %E Cs(Cesium),

%E Sr(Strontium), m *Z f/ 1,9 J 0"

* W Zr, Mo(Molybdenum) _ Fe(Iron) V W

10)" 6. * 3 * k 3(Re _ Mo

kl XY q) _ NpE Yd 2 "

38

E(%) = 100=RD/(1+RD)

S(%) = 100 E

9 R : O/A(volume ratio of organic phase to aqueous phase)

D :)(distribution coefficient : COrg./CAq.)

COrg. :79E < :(mol/L)

CAq. :*79E < :(mol/L)

3.

Re, Np _ UE f _ E ; HLWE 3

]Q d R9 HLW"E E )

(separation factor : DFP/DLLN) 100 7 W[15],

9 %(mixer settler)E + ; 1

+ 70-80% /:, ; v7 ; 60-70% 7,

m 7; 10% $ (7 ) 10/:) V

/Q0" / 6. /;

^ W Q Q; +9 pQ0" T W0

`, +E - E h} Q0" -3

W p$ W6.

3-1.

3-1-1. Re, Np _ U r

Fig. 1 +) 70" NpE Yd(1 g/LE NH4VO3)$

$ 3 30% TBP, O/A=19 XY: d uH Re, Np

_ UE ## W6. ReE Cz NpE Yd

$ v)t XY t O NE VD , X

Y: 1 M D XY: $ u $6$ 1 M

9 - W6. E [11]9 g 5

p XY: 1 M 9 XY : Re T

! TBP :$ T $ W $D, 1 M

79 XY : $ u 7E XY V " B

ReE * ! TBPE :$ 7Q0" -

XY :$ $: b -g 50" }

Re, Np U 39

Eg ,e; E [11, 12]9 g 5p ReE

O (1)p (5) ER, Np _ U;

40

$V ReE r B6. U O XY

: $ u 6 - D - .; m @D ,

5 M9 5% $ fV6. Fig. 1E XY : 2 M

79E U XY : $ u 93-97% /:"

^ Bg6. ,z Np; XY : $ u -` 5 M9

21% /:$ fV6. (2) XY :$ $

T NO3 :$ $V $Vo" -V6.

" ReE PQ 3 U; J$ t0#, Np; 7

fVo" RS g6. R9

B O/A E d /g NpE f -$ V^, I a

ERST w; O/A $34z Npp Re kl $

E kl - 5o" Q S g6.

Fig. 7; XY: _ O/A d uH NpE 6. X

Y: _ O/A $ u - W6. 5 M XY _ O/A=4

9 NpE 6% " - Np fV J

01T W 50" CB6.

Fig. 8; XY: _ O/A d uH ReE 6. X

Y: $ u $`, O/A $ u9 - W6.

+9 -g 5p 1 M 7E XY9 TBP g ReE

r ER, m O/A $ uA ! TBP :

$ ER $ - ^ Bg6. 7E

p" ReE PQ ; 5 M XY, O/A=4 /:z QT

50" +V`, I Re; 80% /: V6.

3-2-3. \ U

Table 2. Separation factor of each element with respected to Np, Re and U

S.F.(DM/DNp) S.F.(DM/DRe) S.F.(DM/DU)

NBA [M] Re/Np Np/Np U/Np HNO3 [M] Re/Re Np/Re U/Re HNO3 [M] Re/U Np/U U/U

0.17 0.5 1.0 13.9 2 1.0 7.7 886 0.01 0.8 0.6 1.00.59 0.7 1.0 15.7 3 1.0 29.4 383 0.05 0.7 0.5 1.01.04 0.9 1.0 16.4 4 1.0 83.8 684 0.1 0.5 0.3 1.01.46 1.4 1.0 25.1 5 1.0 306 690 0.3 0.2 0.1 1.0

Fig. 5. Stripping yields of Np with concentration of normal butyralde-hyde concentration in various O/A ratios.

Fig. 6. Stripping yields of Re, Np and U with nitric acid concentrationat O/A=1.

Fig. 7. Stripping yields of Np with nitric acid concentration in variousO/A ratios.

Fig. 8. Stripping yields of Re with nitric acid concentration in variousO/A ratios.

39 1 2001 2

Re, Np U 41

Fig. 9 O/A=19 XY : d uH Re, Np _ UE f

6. XY : $ u kl - W6. ; XY

:9 TBP g E )$ Q;^[5, 15, 17] B 5

0", 0.05 M HNO39 U, Re _ Np

42

i-

cal

.:

k,

-

ing

m

2,

and

ci-

of

ss-

que-

" pM66. m < E : R

d -,866.

1. OECD Final Report.: Status and Assessment Report on Actinide and

Fission Product Partitioning and transmutation, NEA/PTS/DOC(98)4,

(1998).

2. Takayanagi, M., Fujine, S., Muraoka, S., Kubota, M., Adachi, T.,

Miyoshi, Y., Banba, T., Ohnuki, T. and Sato, T.: Safety Research and

Development of Base Technology on Nuclear Fuel Cycle, JAERI-

Conf 99-004(1999).

3. ICRP report.: Limits for Intake of Radionuclides by Workers, ICRP

Publication, Part I(1978), Part II(1980), Part III(1981).

4. Kondo, Y. and Takitsuka, T.: Technology Assessment of Partitioning

Process, JAERI-M 94-067(1994).

5. Fabienne, W.: Oxydo-Reduction du Np dans les melanges phosphate

tributylique/ dodecane, CEA-R-5478(1989).

6. Lelievre, D., Boussier, H., Grouiller, J. P. and Bush, R. P.: Perspec-

tives and Cost of Partitioning and Transmutation of Long-lived Radio-

nuclides, EUR-17485(1996).

7. Kolarik, Z. and Dressler, P.: Solv. Extr. & Ion Exch., 7(4), 625(1989).

8. Lee, E. H., Kim, K. W., Lim, J. G., Kwon, S. G. and Yoo, J. H.: J.

Korean Ind. & Eng. Chem., 9(2), 232(1998).

9. Benedit, M., Pigford, T. H. and Levi, H. W.: Nuclear Chemical Eng

neering, 2nd Edt., McGraw-Hill Book Company (1981).

10. Tanaka, C., Nemoto, S., Tsubota, T. and Hoshino, T.: Analyti

chemistry of Np, PNCT-841-71-35(1971).

11. Lee, E. H., Kim, K. W., Chung, D. Y., Kwon, S. G. and Yoo, J. H

HWAHAK KONGHAK, 37, 439(1999).

12. Lee, E. H., Lim, J. K., Kim, K. W., Kwon, S. G., Yoo, J. H. and Par

H. S.: HWAHAK KONGHAK, 37, 897(1999).

13. Morita, Y. and Kubota, M.: Recovery of Neptunium, JAERI-M-84

043(1984).

14. Kondo, Y. and Takitsuka, T.: Technology Assessment of Partition

Process, JAERI-M 94-067(1994).

15. Apostolidis, C., Glatz, J. P. and Molinet, R.: Recovery of MA fro

Irradiated SUPERFACT Fuels, Global 1995, Versailles, France,

1027(1995).

16. Pruett, D. J.: The Solvent Extraction of Heptavalent Technetium

Rhenium by Tributyl Phosphate, ORNL/TM-8668(1984).

17. Schulz, W. W., Burger, L. L., Navratil, J. D. and Bender, K. P.: S

ence and Technology of TBP, CRC Press, Ins., Florida, USA(1990).

18. Uchiyama, G., Hotoku, S., Fujine, S. and Maeda, M.: Separation

Np, Pu and U by using Butyraldehydes as Reductants in Reproce

ing, JAERI-M 93-198(1993).

19. Bard, A. J., Parsons, R. and Jordan, J.: Standard Potentials in A

ous Solution, Marcell Dekker, Inc. NewYork, USA(1985).

39 1 2001 2

TBP Re, Np U (2000 6 22 , 2000 11 22 )

A Selective-Separation of Re, Np and Residual U from the Simulated Radwaste Solution Containing t...Eil Hee Lee, Soo Ho Kim, Jae Gwan Lim, Kwang Wook Kim and Jae-Hyung YooKorea Atomic Energy Research Institute (Received 22 June 2000; accepted 22 November 2000)

1. 2. 3. 4.