Recovery. of Actinium-225 and Radium-223 from Natural Thorium Irradiated with Protons

Transcription

1 4 th International Nuclear Chemistry Congress, Maresias, San ulo-brazil, September 14-19, 2014 Recovery of tinium- and dium-223 from Natural orium Irradiated with Protons Elena.V. LAPSHINA, Stanislav V. ERMOLAEV, Boris L. ZHUIKOV, Aleksandr N. VASILIEV, Valentina S. OSTAPENKO, miz A. ALIEV, Stepan N. KALMYKOV Institute for Nuclear Research of Russian ademy of Sciences (Moscow, Russia) Lomonosov Moscow State University, Chemistry Department (Moscow, Russia)

2 and 223 Properties Attractive for Nuclear Medicine q α-rticles have high linear energy transfer (up to 100 kev/µm) and a short pathlength (about µm) in comparison with - particles q and 223 emit four α-particles each in the decay chains providing a higher impact to tumor cells q Intermediate half-lives of and 223 (10.0 d and 11.4 d, respectively) are suitable for manufacturing and therapeutic treatment q and 223 may be also used as generators of the short-lived isotopes: 213 Bi (T 1/2 =46 min) and Pb (T 1/2 =36 min) providing α-particles Slide 2

3 High intensity linear accelerator Isotope production facility Slide 3

4 Main Nuclear Reactions Resulting in and Proton Energy up to 141 MeV INR celerator Capacity for One 10-day Irradiation Run : tivity 2.6 Ci Impurity 0.2 % Decay after EOB 10 days ( ) (p, x) (p, p7n) (8 min, EC, 10%) (p, 4n) 229 (1.4 d, α, 0.48%) (p, x) (14.8 d, β -, 100%) (chemically inseparable impurity) (p, x) Slide 4

5 Main Nuclear Reactions Resulting in 223 and Proton Energy up to 141 MeV INR celerator Capacity for One 10-day Irradiation Run : 223 tivity 4.5 Ci Impurity 16 % Decay after EOB 16 days ( 223 ) (p, p5n) 223 (p, 6n) (38 min, EC, 15%) 224 (chemically inseparable impurity) (p, p4n) (p, 5n) (22 h, EC, 98%) (p, x) (6.1 h, β -, 100%) (18.7 d, α, 100%) 223 (1.91 a, α, 100%) 224 (3.7 d) Slide 5

6 Scheme of 223 Production via 10 Irradiation Decay 8 Optimal decay time tivity, Ci Time, days Slide 6

7 and 223 separation from irradiated Irradiated thorium target dionuclide separation on DGA Resin (N,N,N,, N, -tetroctyldiglicol amide) Dissolution in 6 М HNO 3 with addition of 4*10-3 M HF orium Separation by extraction with tributyl phosphate (TBP), or di(2-ethylhexyl)orthophosphoric acid (HDEHP) dissolved in toluene Water phase,, Ba, Sb, Ce DGA Desorbate 0,01 M HNO 3, La, Ce Organic phase,, Ru, Zr, Nb cumulation 223 from Eluate 4 M HNO 3,, Ba, Cs purification on TRU Resin (octylphenyl-n,n-diisobutylcarbomoylphoshine oxide) - I Purification of fraction - II - Slide 7

8 : Isolation and Purification by Extraction Chromatography DGA Resin TRU Resin 90 Sorption 6 М HNO 3 Sorption and Desorption 2 М HNO 3 80 Desorption 0,01 М HNO La Ce Аctivity, % Column: d=0.35cm, h=8 cm V (TRU Resin) = 0.17 ml/min V, ml Slide 8

9 223 (I): Re-extraction from Organic Phase and Purification TBP HCl HNO 3 Re-extraction, % Ce I Ru Zr Nb Ce I Ru Zr Nb idity, mole/l Water fraction > 99% Ru, I < 1% - may be removed by evaporation with HClO 4 HDEHP Organic fraction Ce, Nb, Zr,,, Ru > 99% Slide 9

10 223 (II): Isolation of from DGA eluate on Dowex-50x8 Column: d=0.8cm, h=7 cm V= 0.5 ml/min 70% H 2 O 0,5 M H 2 SO 4 H 2 O 2 M HNO 3 4 M HNO 3 60% tivity 50% 40% 30% 20% Ru, Sb, Te Te Cs, Be, Ba 223 Cs 136 Ba 140 Ru 103 La 140 Te 123m Be 7 Sb % La 0% Volume, ml Slide 10

11 223 (II): Distribution Coefficients of dium and Barium on Sr Resin (dicyclohexano 18-crown-6 derivative in octanol) E. P. Horwitz, R. Chiarizia and M. L. Dietz, Solvent Extr. Ion Exch. 1992, Vol. 10, pp Slide 11

12 223 (II): Isolation of dium on Sr Resin 60% 50% 40% La Ru 3 M HNO 3 Ba Column: d=0.8cm, h=7 cm V= 0.6 ml/min tivity tivity 30% 20% 10% 0% 60% 50% 40% 30% 20% 10% 0% Volume, ml 0,5 М HClO 4 2 М HNO 3 La, Ru La 140 Ru 103 Ba La 140 Ru 103 Slide 12

13 Scheme of 223 separation I. Solu(on HDEHP in toluene (1:1) a6er liquid- liquid extrac(on 223,224,,, Zr, Nb, Ru Re- extrac(on ( a6er 20 days) 223,224, Ru, I II. Solu(on from DGA Resin, 0,01 M HNO 3 : 223,224, Cs, Ba, La, Sb, Te, Nb, Ag Ca(on exchange resin Dowex 50 х 8 223,224, Ba Separa(on Ru, I by HClO 4 Sorbent Sr- resin Slide 13

14 Conclusions q INR accelerator can provide 2.6 Ci of and 4.5 Ci of 223 during a 10-day irradiation. q diochemical procedures for separation and 223 from spallation and fission products generated in the irradiated thorium target have been developed. q is procedures provide a good chemical yield 80-90% and high radionuclidic purity (99.9%) suitable for medical applications. Slide 14

15 knowledgement e authors are grateful to: q q Dr. Steffen Happel and TrisKem International company for providing the samples of extraction chromatography resins Karpov Institute of Physical Chemistry located in Obninsk for the help in processing thorium targets in hot cells. Slide 15

16 ank you for attention! J 16

17 Вода 17 фракция mg/l Water - frac(on Li <2 <2 Be <0,01 0,033 B 6,9 5,6 Al 0,68 20 V 0,02 0,20 Cr <0,1 10 Mn 0,25 3,7 Co <0.02 0,15 Ni < Cu 0,15 12 Zn 1,0 53 As <0,2 <0,2 Sr <0,05 1,7 Ag 0,045 0,23 Cd <0,01 0,16 Sb 0,023 0,11 Cs <0,01 0,026 Ba 0,14 3,3 Tl <0,005 <0,005 Pb 0,12 18 Bi <0,02 <0,02 <0,02 2,0 U <0,002 0,30

18 Ln Resin M HY MY 3 + 3H + TRU Resin M (NO 3 ) E M(NO 3 ) 3 * E 3 DGA Resin M (NO 3 ) - +3DGA = M(DGA) 3 (NO 3 ) 3 M (NO 3 ) - +2DGA = M(DGA) 2 (NO 3 ) 4 18