Alternative production routes and new separation methods for no-carrier-added 163 Ho
description
Transcript of Alternative production routes and new separation methods for no-carrier-added 163 Ho
Alternative production routes and new separation
methods for no-carrier-added 163HoSusanta 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?
Proton induced reaction
natDy(p,xn) 163Ho σ ~350 mb at 19 MeV
Contributors:
163Dy (24.9%)(p,n)163Ho (σ~0.4 mb)164Dy (28.2%)(p,2n)163Ho (σ~1254 mb)
5 10 15 20 250
100
200
300
400
500
600p+natDy
Ho-163
Ho-162
Projectile Energy [MeV]
Cros
s se
ction
[mb]
Calculations by Maiti et al.
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)158TbRadiochemical separation of 163Ho is recommended! 163Dy(p,a)160TbEnriched target material is preferable!
Calculations by Szucs et al.
Theoretical cross sections of
163Dy(p,n)163Ho and 163Dy(d,2n)163Ho
Calculations by Szucs et al.
Cross section curves of the potential nuclear reactions
5 10 15 20 25 300
100
200
300
400
500
600
700
800
900
1000
163Dy(p,n)163Ho
163Dy(d,2n)163Ho
Energy (MeV)
Cro
ss
se
ctio
n (
mb
)
5 10 15 20 25 300
100
200
300
400
500
600
700
800
900
1000
163Dy(p,n)163Ho
163Dy(d,2n)163Ho
164Dy(p,2n)163Ho
164Er(p,2n) TENDL-2011
164Er(p,x)163Tm exp
Energy (MeV)
Cro
ss
se
ctio
n (
mb
)
Calculations by Szucs et al.
Thick target yields and prices of target materials
Nuclear reaction Energy range [MeV]
Activity [kBq]
thickness [m]
price of target [kUSD]
163Dy(p,n)163Ho 6-14 614 471 1,2 163Dy(p,n)163Ho 2-20 875 1103 2,7 163Dy(d,2n)163Ho 4-20 3600 661 1,6 163Dy(d,2n)163Ho 4-30 5000 1350 3,3 164Dy(p,2n)163Ho 8,5-30 9800 2000 4,9 164Er(p,2n)163Tm 10,7-28,7 12000* 1620 61,9
*reached by decay chain of 163Tm 163Er 163Ho
Calculations by Szucs et al.
Contaminating isotopes
-10.0 10.0 30.01E-02
1E+01
1E+04
Energy (MeV)
Cro
s
s
se
cti
on
(mb
)
0.0 5.0 10.0 15.0 20.0 25.0 30.01E-02
1E-01
1E+00
1E+01
1E+02
1E+03
natDy(p,x)158Tb
natDy(p,x)157Tb cum
natDy(p,x)159Dy
natDy(p,x)163Ho
164Dy(p,g)165Ho
Energy (MeV)
Cro
ss s
ecti
on (
mb
)
Calculations by Szucs et al.
Irradiation of natDy by proton
Energy 163Ho 157Tb 158Tb 159Dy
range [MeV] [MBq] [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
Calculations by Szucs et al.
Comments
1. The highest yield give the (p,2n) reaction2. 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 contamination4. 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.
p+ Dy2O3
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.
-induced reactions
natDy(α, xn) 163Er () 163HoCalculations by Maiti et al.
+Dy2O3
10 15 20 25 30 35 40 45 500
100
200
300
400
500
600+natDy
Er-165, 10.3hEr-163, 75mEr-161, 3.24hEr-160, 28.6h
Energy, MeVCr
oss
seci
on, m
b
natDy(α, xn) 163Er () 163Ho(σ ~500 mb at 40 MeV)
Irradiation parameters:
Projectile : α EP = 40 MeVfirst target: 1 µA, 7 h irradiation second target: 3 µA, 11 h irradiation
Exhaustive Chemistry !!Experiment and Calculations by Maiti et al.
RadioChemical Separation of Er and Dy
0.1 0.2 0.3 0.4 0.50
20
40
60
80
100
at 1% HDEHP
DyEr
[HCl], M
Extr
actio
n, %
161Er was used as monitor of Er in the radiochemical separation
&Dy was measured by ICP-OES
Technique – Liquid liquid extraction Reagents: di-(2-ethylhexyl) phosphoric acid (HDEHP) dissolved in cyclohexane (Organic phase) & HCl (aqueous phase)
HCl : 0.2 M & HDEHP 1%Extraction: Dy 48.8%
Er 84%
Separation scheme
Experiment by Maiti et al.
Li-induced reaction
159Tb(7Li, 3n) 163Er (σ ~312 mb at 31 MeV)
25 30 35 400
200
400
600
800
1000
12007Li+159Tb
163 Er
Energy [MeV]
Cros
s se
ction
[mb]
Calculations by Maiti et al.
Irradiation
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
Calculation for natDy(p,xn) reaction:
For a sample thickness: 4 mg/cm2
No. of 163Ho (via 163Er) will be = 2.5x1010 atoms/A-h
For enriched target it will increase by factor of 2.
For 10 A, 100 h irradiation (one target): 2.5 x 1013 atoms
Maiti et al.
Calculation for Dy(,xn) reaction:
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
Maiti et al.
Calculation for 159Tb(7Li,3n) reaction:
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
Maiti et al.
Consequences!
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 CollaborationThis 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 use4. Development of new separation techniques based
on HPLC