Alternative production routes and new separation methods for nocarrier-added 163Ho Susanta Lahiri, Moumita Maiti Saha Institute of Nuclear Physics, Kolkata, India & Zoltán Szűcs, Sandor Takacs Institute of Nuclear Research of H.A.S. Debrecen, Bem tér 18/C HUNGARY 163Ho: How to produce? p+natDy 600 σ ~350 mb at 19 MeV 500 Contributors: Cross section [mb] natDy(p,xn) 163Ho 400 Ho-163 Ho-162 300 Ho-161 Ho-160 200 100 163Dy (24.9%)(p,n)163Ho (σ~0.4 mb) 164Dy (28.2%)(p,2n)163Ho (σ~1254 mb) 0 5 10 15 20 Projectile Energy [MeV] 25 Main reaction: 163Dy(p,n)163Ho Side reactions: 158Dy)p,2n)157Ho→157Dy→157Tb 160Dy(p,2n)159Ho→159Dy 160Dy(p,2p)159Dy 156Dy(p,3n)154Ho→154Dy 161Dy(p,a)158Tb 163Dy(p,a)160Tb Radiochemical separation of 163Ho is recommended! Enriched target material is preferable! Theoretical cross sections of 163Dy(p,n)163Ho and 163Dy(d,2n)163Ho Cross section curves of the potential nuclear reactions 1200 163Dy(p,n)163Ho 1200 163Dy(p,n)163Ho 163Dy(d,2n)163Ho 1000 1000 Cross section (mb) 800 164Dy(p,2n)163Ho 163Dy(d,2n)163H o 164Dy(p,2n)163H o 800 Cross section (mb) 600 164Er(p,2n) TENDL-2011 400 164Er(p,x)163Tm exp 600 200 0 0 400 5 10 15 Energy (MeV) 20 25 30 200 0 0 5 10 15 Energy (MeV) 20 25 30 Thick target yields and prices of target materials Nuclear reaction 163 Dy(p,n)163Ho 163 Dy(p,n)163Ho 163 Dy(d,2n)163Ho 163 Dy(d,2n)163Ho 164 Dy(p,2n)163Ho 164 Er(p,2n)163Tm Energy range [MeV] 6-14 2-20 4-20 4-30 8,5-30 10,7-28,7 *reached by decay chain of 163Tm Activity [kBq] 614 875 3600 5000 9800 12000* 163 Er 163 Ho thickness [m] 471 1103 661 1350 2000 1620 price of target [kUSD] 1,2 2,7 1,6 3,3 4,9 61,9 Contaminating isotopes 1.E+02 1.E+01 1.E+00 natDy(p,x)158Tb 1.E+03 1.E-02 -20.0 Energ… Cr… Cross section (mb) 1.E+03 natDy(p,x)157Tb cum natDy(p,x)159Dy 1.E-01 natDy(p,x)163Ho 164Dy(p,g)165Ho 1.E-02 0.0 5.0 10.0 15.0 20.0 Energy (MeV) 25.0 30.0 Irradiation of natDy by proton Energy 163Ho range [MeV] [MBq] 157Tb 158Tb 159Dy [MBq] [MBq] [MBq] 5-11 0,20 0,00 0,00 0 5-18 1,74 3,81 0,04 968 5-28.7 2,93 18,27 1,10 20732 1. The highest yield give the (p,2n) reaction 2. Er irradiation is NOT preferred because of the side reactions, producing the stable 165Ho as well as the radioactive 166Ho!!!! 3. The enriched target of 164Dy has to be used. In other case during the irradiation of the natDy the 157-158Tb and 159Dy will give us extremely high contamination 4. During the irradiation of enriched 164Dy we will get the stable 165Ho too by the 164Dy(p, γ)165Ho reaction. However this amount is 2 magnitude less, than 163Ho. 5. The calculation of cross section curve of 157Tb contains all possible reaction for 157Ho, 157Dy and 157Tb, as well as for 159Dy also contains all possible reaction for 159Ho and 159Dy. 6. Due to the 10 times higher yield of the (p,2n) reaction than the (p,n) reaction not necessary 1800 hours irradiation time to get 1 MBq 163Ho, approximately. Looks that is enough 180 hours, 10 times less, therefore the irradiation cost in cyclotron also can be 10 times less, it means that is 50kEuro, approximately, which is comparable with the irradiation on reactor!!!!! 7. The Debrecen cyclotron can't produce the 30MeV proton beam. Irradiation Parameters: (i) Projectile – p, (ii) Ep = 19 MeV, (iii) current: 700 nA, (iv) time of irradiation: 10 h Two targets were irradiated in stack with the following configuration There is no way to monitor Ho-163 by monitoring its nuclear properties. Separation of Dy and Ho is difficult. Very long time is required to rich the saturation activity. natDy(α, xn) 163Er () 163Ho Er-165, 10.3h Er-163, 75m Er-161, 3.24h Er-160, 28.6h Ho-163, 4750y a+natDy 600 Projectile : α EP = 40 MeV first target: 1 µA, 7 h irradiation second target: 3 µA, 11 h irradiation 500 Cross secion, mb Irradiation parameters: 400 300 200 100 0 10 15 20 25 30 35 40 Energy, MeV natDy(α, xn) 163Er () 163Ho (σ ~500 mb at 40 MeV) Exhaustive Chemistry !! 45 50 Technique – Liquid liquid extraction Reagents: di-(2-ethylhexyl) phosphoric acid (HDEHP) dissolved in cyclohexane (Organic phase) & HCl (aqueous phase) 161Er was used as monitor of Er in the radiochemical separation & Dy was measured by ICP-OES 100 Extraction, % 80 60 Dy 40 Er 20 HCl : 0.2 M & HDEHP 1% Extraction: Dy 48.8% Er 84% at 1% HDEHP 0 0.1 0.2 0.3 [HCl], M 0.4 0.5 159Tb(7Li, 3n) 163Er (σ ~312 mb at 31 MeV) Cross section [mb] 1200 7Li+159Tb 1000 800 600 163 Er 400 162 Er 200 0 25 30 35 Energy [MeV] 40 Irradiation parameters: (i) Projectile – 7Li (ii) EP = 31 MeV (iii) current: 150 nA (iv) time of irradiation: 11 h No successful results have been achieved using HDEHP For a sample thickness: 4 mg/cm2 No. of 163Ho (via atoms/A-h 163Er) will be = 2.5x1010 For enriched target it will increase by factor of 2. For 10 A, 100 h irradiation (one target): 2.5 x 1013 atoms For a sample thickness: 4 mg/cm2 No. of 163Ho (via 163Er) will be = 2x1010 atoms/A-h In 6 h, irradiation time = 1.2x1011 atoms 20 A current, 5 targets in a row, 6 h irradiation time 1.2 x 1013 atoms For a sample thickness: 4 mg/cm2 No. of 163Ho (via 163Er) will be = 4x109 atoms/A-h In 6 h, irradiation time = 2.4x1010 atoms 20 A current, 5 targets in a row, 6 h irradiation time 2.4 x 1012 atoms 163Ho can be produced by charged particle activation through direct or indirect way However, separation of Ho from the target matrix is extremely difficult due to the similar chemical properties of lanthanides Therefore, it needs special attention towards the purification procedure In order to ensure the production of 163Ho nuclear properties can not be exploited as it behaves like stable isotope ECHo Collaboration This collaboration has been formed on 29th June, 2012 Participants: 10 Institutes from 5 countries Thank you…. Future Plan from SINP and ATOMKI Group 1. Will apply for beam time in VECC, Kolkata and in Atomki, Hungary 2. Verification of theoretical data as much as possible. 3. Storing Ho-163 for future use 4. Development of new separation techniques based on HPLC