Alternative production routes and new separation methods for no-carrier-added 163 Ho

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Alternative production routes and new separation methods for no-carrier-added 163 Ho 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
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Alternative production routes and new separation methods for no-carrier-added 163 Ho. 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. - PowerPoint PPT Presentation

Transcript of Alternative production routes and new separation methods for no-carrier-added 163 Ho

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Alternative production routes and new separation methods for no-carrier-added 163HoSusanta Lahiri, Moumita MaitiSaha Institute of Nuclear Physics, Kolkata, India&Zoltn Szcs, Sandor TakacsInstitute of Nuclear Research of H.A.S.Debrecen, Bem tr 18/CHUNGARY163Ho: How to produce?

Proton induced reactionnatDy(p,xn) 163Ho ~350 mb at 19 MeV

Contributors:

163Dy (24.9%)(p,n)163Ho (~0.4 mb)164Dy (28.2%)(p,2n)163Ho (~1254 mb)

Calculations by Maiti et al.

Main reaction: 163Dy(p,n)163HoSide reactions: 158Dy)p,2n)157Ho157Dy157Tb 160Dy(p,2n)159Ho159Dy 160Dy(p,2p)159Dy 156Dy(p,3n)154Ho154Dy 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 reactionsCalculations by Szucs et al. Thick target yields and prices of target materials

Calculations by Szucs et al. Contaminating isotopesCalculations by Szucs et al. Irradiation of natDy by protonEnergy163Ho157Tb158Tb159Dyrange [MeV][MBq][MBq][MBq][MBq]5-110,200,000,0005-181,743,810,049685-28.72,9318,271,1020732Calculations by Szucs et al. CommentsThe highest yield give the (p,2n) reactionEr irradiation is NOT preferred because of the side reactions, producing the stable 165Ho as well as the radioactive 166Ho!!!!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 contaminationDuring the irradiation of enriched 164Dy we will get the stable 165Ho too by the 164Dy(p, )165Ho reaction. However this amount is 2 magnitude less, than 163Ho. 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.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!!!!!The Debrecen cyclotron can't produce the 30MeV proton beam.p+ Dy2O3Irradiation Parameters: (i) Projectile p, (ii) Ep = 19 MeV, (iii) current: 700 nA, (iv) time of irradiation: 10 hTwo 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(, xn) 163Er () 163Ho

Calculations by Maiti et al.+Dy2O3natDy(, xn) 163Er () 163Ho( ~500 mb at 40 MeV)Irradiation parameters: Projectile : EP = 40 MeVfirst target: 1 A, 7 h irradiation second target: 3 A, 11 h irradiationExhaustive Chemistry !!Experiment and Calculations by Maiti et al.RadioChemical Separation of Er and Dy161Er was used as monitor of Er in the radiochemical separation&Dy was measured by ICP-OESTechnique Liquid liquid extractionReagents: 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 ( ~312 mb at 31 MeV)Calculations by Maiti et al.IrradiationIrradiation 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 HDEHPCalculation 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/cm2No. 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, 2012Participants: 10 Institutes from 5 countriesThank you.

Future Plan from SINP and ATOMKI GroupWill apply for beam time in VECC, Kolkata and in Atomki, HungaryVerification of theoretical data as much as possible. Storing Ho-163 for future useDevelopment of new separation techniques based on HPLC Diagram10.004171330.04757020.4064870.8619124.111546.7940230.241231.14486.952393.455232.112195.173452.474236.305661.44133.353835.4278.5778887.65655.2736784.55946.3795643.09443.2763524.21342.2969435.12941.728368.56641.3466318.13640.9965280.56540.5858

DeuteronProtonEnergy [MeV]Cross section [mbarn]

Sheet1Reaction:# d + 163Dy: Production of 163Ho - Total# p + 163Dy: Production of 163Ho - Totalunit = 1uCi/uAh9.73E-08produced isotope163Hosat. yield = phys. yield / lambda# Q-value =-3.00948E+00 mass= 162.928733# Q-value =-7.84909E-01 mass= 162.928733unit = 2mCi/uAh9.73E-11half life h400606201Ci=3.7E+10Bq# E-threshold= 3.04667E+00# E-threshold= 7.89762E-01unit = 3Bq/uAh3.60E-03target molmass g164.9301C=6.2414601E18es=1As# # energies = 45# # energies = 45unit = 4kBq/uAh3.60E-06target ro g/cm38.550602204500000000000000000Av# E xs# E xsunit = 5MBq/uAh3.60E-09Z number of particle119.2900584795for micron1010unit = 6kBq/C1.00E-03E-in (MeV)19.90.016493g/cm22020.00000027unit = 7MBq/C1.00E-06E-out (MeV)260220450000000000000atom/cm23030.000588227unit = 8GBq/C1.00E-09irradiation time h180022.41l/mol40.004171330.047570240.0475702unit = 1uCi9.73E-08target ratio124l/mol20C1atm50.4064870.86191250.861912unit = 2mCi9.73E-11beam current uA2064.111546.7940266.79402unit = 3Ci9.73E-14lambda 1/h0.0000000173730.241231.144731.144unit = 4Bq3.60E-03Norm. const0.0936486949886.952393.455893.455unit = 5kBq3.60E-060.00000360.00000000013.60E-069232.112195.1739195.173unit = 6MBq3.60E-09unit 1kBq/uAh410452.474236.30510236.305unit = 7GBq3.60E-12unit 2mCi/uAh211661.44133.35311133.353unit = 8unit 3kBq512835.4278.57781278.5778Na2AsO40PhysicalPhys. yieldPhys. yieldfixed timesat. yield13887.65655.27361355.2736EnergyRangedx inEnergysigmaInt yieldkBq/uAhmCi/uAhkBqkBq14784.55946.37951446.3795mevmicronmicronmevmbarnBq/C0.0240.000862.52769342915643.09443.27631543.27630.11.141.120.114.06.66E+030.0240.000862.52769342916524.21342.29691642.29690.21.90.760.00E+00000.000.0017435.12941.7281741.7280.32.750.850.00E+00000.000.0018368.56641.34661841.34660.43.730.980.00E+00000.000.0019318.13640.99651940.99650.54.821.090.00E+00000.000.0020280.56540.58582040.58580.66.021.20.00E+00000.000.000.77.321.30.00E+00000.000.000.88.71.380.00E+00000.000.000.910.161.460.00E+00000.000.00111.71.540.00E+00000.000.00163Dy3.6USD/mg1.113.281.580.00E+00000.000.00500 mg 163Dy1800USD/mg1.214.941.660.00E+00000.000.001.316.661.720.00E+00000.000.001.418.461.80.00E+00000.000.001.520.321.860.00E+00000.000.00EnergyDeuteronProton1.622.241.920.00E+00000.000.0040.004171330.04757021.724.231.990.00E+00000.000.0050.4064870.8619121.826.282.050.00E+00000.000.0064.111546.794021.928.392.110.00E+00000.000.00730.241231.144230.562.172.00.00.00E+00000.000.00886.952393.4552.132.82.242.10.05.87E-05000.000.249232.112195.1732.235.092.292.20.01.75E-04000.000.7310452.474236.3052.337.432.342.30.03.45E-04000.001.4411661.44133.3532.439.842.412.40.05.67E-04000.002.3612835.4278.57782.542.312.472.50.08.28E-04000.003.4513887.65655.27362.644.822.512.60.01.11E-03000.004.6314784.55946.37952.747.42.582.70.01.40E-03000.005.8515643.09443.27632.850.032.632.80.01.68E-03000.006.9816524.21342.29692.952.712.682.90.01.91E-03000.007.9317435.12941.728355.452.743.00.02.06E-03000.008.5618368.56641.34663.158.242.793.10.02.11E-03000.008.7719318.13640.99653.261.092.853.20.02.11E-03000.008.7820280.56540.58583.363.992.93.30.02.21E-03000.009.213.466.942.953.40.02.67E-03000.0011.123.569.9433.50.03.85E-03000.0016.013.672.993.053.60.06.21E-03000.0025.863.776.13.113.70.01.04E-02000.0043.253.879.253.153.80.01.71E-02000.0071.093.982.463.213.90.02.72E-02000.00113.17485.713.254.00.04.17E-02000.01173.424.189.013.34.10.16.18E-02000.01257.354.292.373.364.20.18.99E-02000.01374.174.395.773.44.30.11.29E-01000.02536.364.499.233.464.40.21.83E-01000.02762.614.5102.733.54.50.22.58E-01000.031074.054.6106.283.554.60.33.60E-01000.051498.764.7109.883.64.70.44.97E-01000.062069.354.8113.533.654.80.56.79E-01000.092823.904.9117.233.74.90.79.15E-01000.123806.145120.983.755.00.91.22E+00000.165065.705.1124.773.795.11.11.60E+00000.216656.865.2128.613.845.21.32.08E+00000.278661.445.3132.493.885.31.72.69E+00000.3511175.285.4136.423.935.42.13.44E+00000.4514330.545.5140.393.975.52.54.39E+00000.5718270.195.6144.414.025.63.15.57E+00000.7223181.795.7148.464.055.73.87.03E+00000.9129243.035.8152.574.115.84.78.83E+00001.1436732.295.9156.734.165.95.71.10E+01001.4345901.076160.954.226.06.81.37E+01001.7857073.556.1165.24.256.18.11.69E+01002.2070497.286.2169.54.36.29.62.08E+01002.7086600.146.3173.844.346.311.32.54E+01003.29105760.056.4178.224.386.413.33.09E+01004.00128432.676.5182.644.426.515.53.73E+01004.83155121.076.6187.114.476.618.04.48E+01005.81186447.176.7191.624.516.720.85.36E+01006.94222953.636.8196.174.556.823.96.38E+01008.26265295.026.9200.774.66.927.37.55E+01009.79314285.177205.424.657.031.18.91E+010011.55370715.237.1210.124.77.135.31.05E+020013.56435437.597.2214.864.747.239.91.22E+020015.86509217.147.3219.644.787.345.01.43E+020018.47593006.617.4224.464.827.450.51.65E+020021.42687826.767.5229.324.867.556.51.91E+020024.75794767.997.6234.234.917.663.02.20E+020028.50915237.277.7239.174.947.770.02.52E+020032.701049978.307.8244.164.997.877.62.89E+020037.401200847.587.9249.185.027.985.83.29E+020042.621368625.178254.255.078.094.63.74E+020048.441555444.238.1259.365.118.1104.04.24E+020054.891762458.608.2264.515.158.2113.94.78E+020062.011990954.178.3269.725.218.3124.15.39E+020069.852242918.038.4274.965.248.4134.66.05E+020078.412517684.968.5280.265.38.5145.16.77E+020087.742817330.568.6285.595.338.6155.57.55E+020097.803140367.268.7290.955.368.7165.78.38E+0200108.593486579.268.8296.365.418.8175.69.27E+0200120.123856811.368.9301.815.458.9185.01.02E+0300132.354249649.949307.35.499.0193.71.12E+0300145.264663997.749.1312.835.539.1201.61.23E+0300158.795098437.859.2318.45.579.2208.61.33E+0300172.895551301.699.33245.69.3214.71.45E+0300187.486019845.249.4329.655.659.4219.71.56E+0300202.556503590.169.5335.335.689.5223.61.68E+0300217.966998426.979.6341.075.749.6226.21.80E+0300233.717504322.079.7346.855.789.7227.41.93E+0300249.678016609.399.8352.685.839.8227.32.05E+0300265.758532983.719.9358.545.869.9225.62.17E+0300281.809048209.7410364.445.910.0222.32.30E+0300297.729559430.8910.1370.375.9310.1217.42.42E+0300313.3710061902.3010.2376.355.9810.2211.12.54E+0300328.6910553782.7710.3382.376.0210.3203.52.65E+0300343.5511031192.9710.4388.426.0510.4195.02.76E+0300357.8711490860.3810.5394.516.0910.5185.72.87E+0300371.6011931602.4810.6400.646.1310.6176.02.97E+0300384.6912351992.2810.7406.816.1710.7166.03.06E+0300397.1212751166.6410.8413.026.2110.8156.13.16E+0300408.8813128841.4910.9419.266.2410.9146.43.24E+0300419.9713484756.5411425.546.2811.0137.23.32E+030.010430.4213820437.5611.1431.866.3211.1128.73.40E+0300440.2914137308.2511.2438.236.3711.2120.93.47E+0300449.6314437308.2911.3444.656.4211.3113.73.54E+0300458.4914721777.0211.4451.16.4511.4107.23.60E+0300466.8814991149.3211.5457.596.4911.5101.23.66E+0300474.8615247110.2111.6464.126.5311.695.83.72E+0300482.4515490819.7811.7470.696.5711.790.83.78E+0300489.6915723353.6211.8477.296.611.886.33.83E+0300496.6015945363.7511.9483.936.6411.982.23.88E+0300503.2316158101.1412490.616.6812.078.53.93E+0300509.5916362370.5312.1497.326.7112.175.03.98E+0300515.7016558599.4512.2504.076.7512.271.94.02E+0300521.5916747766.6212.3510.876.812.369.14.07E+0300527.2916930777.0912.4517.76.8312.466.54.11E+0300532.8017107690.4412.5524.556.8512.564.14.15E+0300538.1317278834.5412.6531.456.912.662.04.19E+0300543.3217445485.1812.7538.396.9412.760.04.23E+0300548.3817607867.9112.8545.376.9812.858.34.27E+0300553.3217766415.2312.9552.387.0112.956.74.31E+0300558.1417921294.7113559.437.0513.055.24.34E+0300562.8718073076.1513.1566.537.113.153.94.38E+0300567.5118222271.4713.2573.667.1313.252.74.41E+0300572.0718368742.3913.3580.847.1813.351.64.45E+0300576.5718513167.2813.4588.057.2113.450.64.48E+0300581.0018655395.7113.5595.37.2513.549.74.52E+0300585.3818795864.8913.6602.597.2913.648.94.55E+0300589.7018934794.7513.7609.917.3213.748.24.58E+0300593.9819072200.8313.8617.277.3613.847.54.62E+0300598.2319208459.5813.9624.667.3913.946.94.65E+0300602.4319343556.5414632.097.4314.046.44.68E+0300606.6219477826.9814.1639.567.4714.145.94.71E+0300610.7819611404.6514.2647.067.514.245.44.74E+0300614.9119744237.1314.3654.617.5514.345.14.78E+0300619.0419876796.1414.4662.187.5714.444.74.81E+0300623.1520008666.2214.5669.87.6214.544.44.84E+0300627.2520140473.5714.6677.447.6414.644.14.87E+0300631.3420271794.6414.7685.127.6814.743.94.90E+0300635.4320403061.4914.8692.847.7214.843.64.93E+0300639.5220534352.0714.9700.67.7614.943.44.97E+0300643.6120665735.8815708.397.7915.043.35.00E+0300647.7020797105.1915.1716.217.8215.143.15.03E+0300651.8020928513.9915.2724.087.8715.243.05.06E+0300655.9021060345.7715.3731.987.915.342.95.09E+0300660.0121192308.1315.4739.917.9315.442.85.12E+0300664.1321324439.7415.5747.877.9615.542.75.16E+0300668.2521456774.2115.6755.888.0115.642.65.19E+0300672.3921589671.7615.7763.938.0515.742.55.22E+0300676.5421722988.7115.8772.028.0915.842.45.25E+0300680.7121856742.3815.9780.158.1315.942.45.28E+0300684.8821990944.7016788.318.1616.042.35.32E+0300689.0722125437.2516.1796.518.216.142.25.35E+0300693.2822260386.9916.2804.758.2416.242.25.38E+0300697.4922395795.3316.3813.028.2716.342.15.41E+0300701.7222531500.0916.4821.338.3116.442.05.45E+0300705.9622667668.2016.5829.668.3316.542.05.48E+0300710.2122803975.4816.6838.038.3716.641.95.51E+0300714.4722940753.4416.7846.448.4116.741.95.55E+0300718.7423078006.3716.8854.898.4516.841.85.58E+0300723.0323215739.2616.9863.378.4816.941.85.61E+0300727.3323353794.9317871.898.5217.041.75.65E+0300731.6423492342.5617.1880.438.5417.141.75.68E+0300735.9623631063.9717.2889.028.5917.241.65.71E+0300740.3123770452.8117.3897.648.6217.341.65.75E+0300744.6623910190.0317.4906.38.6617.441.65.78E+0300749.0324050442.6217.5914.998.6917.541.55.81E+0300753.4024191052.7917.6923.718.7217.641.55.85E+0300757.8024332024.0017.7932.468.7517.741.45.88E+0300762.2024473359.0617.8941.258.7917.841.45.92E+0300766.6124615221.2917.9950.088.8317.941.45.95E+0300771.0524757611.5418958.948.8618.041.35.98E+0300775.5024900368.7618.1967.848.918.141.36.02E+0300779.9625043653.4918.2976.778.9318.241.36.05E+0300784.4325187303.7818.3985.738.9618.341.26.09E+0300788.9225331318.4118.4994.73918.441.26.12E+0300793.4225475856.4318.51003.779.0418.541.26.16E+0300797.9425620915.6118.61012.849.0718.641.16.19E+0300802.4725766333.1218.71021.949.118.741.16.23E+0300807.0125912106.2518.81031.089.1418.841.16.26E+0300811.5626058392.0618.91040.259.1718.941.06.30E+0300816.1326205026.90191049.449.1919.041.06.33E+0300820.7026351847.1919.11058.699.2519.141.06.37E+0300825.3026499487.6219.21067.969.2719.240.96.40E+0300829.9026647305.5619.31077.279.3119.340.96.44E+0300834.5226795616.2919.41086.619.3419.440.86.48E+0300839.1526944257.1119.51095.999.3819.540.86.51E+0300843.7927093383.9819.61105.49.4119.640.86.55E+0300848.4527242835.1419.71114.849.4419.740.76.58E+0300853.1127392608.2219.81124.329.4819.840.76.62E+0300857.7927542859.7819.91133.839.5119.940.66.66E+0300862.4827693429.42

Sheet1

Energy (MeV)Cross section (mb)

DeuteronProtonEnergy [MeV]Cross section [mbarn]Production of 163Ho by cyclotron