Modeling and experimental data of zirconium-89 production yield

Author’s Accepted Manuscript Modeling and experimental data of zirconium-89 production yield Mozhgan Sharifian, Mahdi Sadeghi, Behrouz Alirezapour, Mohammad Yarmohammadi, Khosro Ardaneh www.elsevier.com/locate/apradiso

PII: DOI: Reference:

S0969-8043(17)30838-2 https://doi.org/10.1016/j.apradiso.2017.09.044 ARI8095

To appear in: Applied Radiation and Isotopes Received date: 10 July 2017 Revised date: 16 September 2017 Accepted date: 28 September 2017 Cite this article as: Mozhgan Sharifian, Mahdi Sadeghi, Behrouz Alirezapour, Mohammad Yarmohammadi and Khosro Ardaneh, Modeling and experimental data of zirconium-89 production yield, Applied Radiation and Isotopes, https://doi.org/10.1016/j.apradiso.2017.09.044 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting galley proof before it is published in its final citable form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

Modeling and experimental data of zirconium-89 production yield

Mozhgan Sharifiana, Mahdi Sadeghi b*, Behrouz Alirezapourc, Mohammad Yarmohammadic, Khosro Ardanehc

a

b

Department of Physics, Payame Noor University, P.O. Box: 19395-3697, Tehran, Iran,

Medical physics department, School of Medicine, Iran University of Medical Science, P.O. Box: 14155-6183,Tehran, Iran c

Radiation Application Research School, Nuclear Science and Technology Research Institute, P.O. Box: 14395-836, Tehran, Iran, *Corresponding Author, E-mail: [email protected]

Abstract The radionuclide zirconium-89 can be employed for the positron emission tomography (PET). In this study 89Zr excitation function via

89

Y(p,n)89Zr reaction was calculated by the

TALYS-1.8 code based on microscopic level density model. The formation of

89

Zr was

simulated using the Monte Carlo simulation code MCNPX to calculate the integral yield in the 89Y target body for threshold up to 40 MeV incident-proton energy. The target thickness was based on calculation of the stopping power using the SRIM-2013 code matched to any incident-proton energy. The production yield of the method for the

89

Y(p,n)89Zr,

89

89

Zr simulated with the Monte Carlo

Y(d,2n)89Zr, natSr(α,xn)89Zr and

nat

Zr(p,pxn)89Zr reactions and

the results were in good agreement with published experimental results for the optimum energy range. An experimental yield of 53.1 MB/µA for the 15 MeV proton-induced on Y2O3 powder as a disk-target obtained for 1 hour irradiation at the AMIRS cyclotron.

1

Key words: Monte Carlo; Integral yield; Radionuclide; Zirconium-89.

1. Introduction

It is possible to employ radionuclide zirconium-89 (T1/2 = 78.41 h; IEC = 76.6%; Iβ+ = 22.3%; Emax

(β +)

= 897 keV, Eave (β +) = 397 keV; Eγ = 908.9 keV; Iγ = 100%) in positron emission

tomography (PET) because of its suitable half-life, emission of low energy positrons, suitable branching ratio for positron emission and emission of significant gamma radiation (Wooten, et al., 2013). Methods for accelerator production of nat

89

Zr include

89

Y(p,n)89Zr,

89

Y(d,2n)89Zr,

Sr(α,xn)89Zr, natZr(p,pxn)89Zr and 90Zr(n,2n)89Zr (Sadeghi, et al., 2010; Sadeghi, et al., 2011;

Omara, et al., 2009; Khandaker, et al., 2012; Zweit, et al., 1991; Kandil, et al., 2007; Uddin, et

al., 2008). Yttrium is a monoisotopic element therefore is an ideal target material to test nuclear reaction (Satheesh, et al., 2011). The

89

Y(p,n)89Zr reaction was investigated for

possible use because it offers several advantages (Sadeghi, et al., 2012). The calculated optimal range of energy and no-carrier-added

89

Zr makes it ideal for low-energy cyclotrons

(Dabkowski, et al., 2012). The simulation is fundamental to the domains of experimental production and the Monte Carlo simulation method can decrease the expense, facilitate analysis and save time by optimization of production. The target geometry, target thickness, optimal range of energy and activity of production of radionuclides are the significant parameters for the production of 89Zr (Sharifian, et al., 2017a). In this study the excitation function was calculated to illustrate the formation of zirconium radionuclide through the reaction of

89

Y(p,n)89Zr. TALYS-1.8 (Koning, et al., 2015) code

was used to calculate the excitation function and the optimum energy range determined. The stopping power and target thickness for all ranges of incident energy were obtained using the stopping power and range of ions in matter (SRIM) code (Ziegler, 2013). The production yield was calculated based on stopping power for 5-40 MeV incident proton energy on the 2

yttrium target. Then the integral yield simulated using MCNPX code (Monte Carlo Team, https://mcnpx.lanl.gov//) and the result were compared with experimental data. In Particular,

we concentrated on the production of

89

Zr using Yttrium Oxide-powder as a target at the

AMIRS cyclotron by 15 MeV proton beam energy.

2. Materials and methods 2.1. Calculation of excitation function The TALYS-1.8 code exploited and the optimum energy range determined to demonstrate the formation of zirconium radionuclide. TALYS-1.8 is the newest version of the TALYS computer code and contains the simulation of nuclear reactions for incident particles such as protons, neutrons, photons, deuterons, tritons, 3He and alpha-particles and for target nuclei from Li nucleus to Dy nucleus in the 0.01 keV to 200 MeV incident particle energy range (Koning, et al., 2015). Also, the TALYS code provides a complete description of all the reaction channels and observables of the reaction (Sadeghi, et al., 2009; Mirzaii et al., 2010). Surely data on nuclear level densities are crucial input parameters in calculating the nuclear cross-sections of the reactions (Yiğit, et al., 2016). The cross sections for some reactions have been calculated using the ALICE code based on level density model by Yiğit (Yiğit, et al., 2015). According to our previous work, the excitation function based on HFB model using the TALYS-1.8 code for the

89

Y(p,n)89Zr reaction has the best overall agreement with

experimental data (Sharifian et al., 2017b). The HFB model from Hilaire's combinatorial tables (temperature dependent, Gogny force), is a microscopic level density model (Koning et al., 2008). Therefore, to achieve the best computational result, this model has been employed to calculate the cross-section by TALYS-1.8 code.

2.2. Theoretical yield

3

SRIM code was used to estimate the stopping power in the target. The production yield of radionuclide was calculated using the excitation function (Qaim, 2011) as: (

)∫ (

(

)

)

( )

( )

where Y is the activity (in Bq) of the product, L is the Avogadro number, H is the isotope abundance of the target nuclide, M is the mass number of the target element, σ(E) is the cross-section at energy E, I is the projectile current, dE/d(ρx) is the stopping power, λ is the decay constant of the product, and t is the time of irradiation. The production yield of using

89

89

Zr

Y(p,n)89Zr and the other reactions were calculated using the Simpson numerical

integral.

2.3. MCNPX code MCNPX-2.6 is a general-purpose Monte Carlo radiation transport code. This code was developed and is authorized by the Los Alamos National Laboratory. MCNPX was designed to track different particle types over a broad range of energies and to analyze the transport of neutrons, protons, gamma rays and other particles (Bakht, et al., 2012). MCNPX includes many new capabilities, particularly in the areas of transmutation and delayed particle production. In addition, new tally sources and variance-reduction options have been developed. In particular, this code can be used to simulate the irradiation of target materials with charged hadrons to optimize the target design and study the activation of the materials. The MCNPX input file formed by the geometry, the materials introduction, the tallies type and the techniques of variance reduction.

2.3.1. Target geometry Several techniques have been used to make yttrium target materials for proton bombardment in a cyclotron. These include yttrium stacked foils, yttrium pellets and electroplated yttrium 4

targets. In the present work, the yttrium powder was simulated in the cylinder form assembled in an aluminum target boat. The designed target and source are shown in Fig. 1. The target consists of the objective element cylinder (radius = 5 mm; thickness = 1 mm) and the source simulated by the proton beam with 15 MeV of energy around the Z axis in a negative direction. The simulated proton beam had a Gaussian profile and full width at half maximum (FWHM) values of 5.3 and 4.2 mm in the x- and y-directions, respectively. The target thickness can be changed to the compatible incident energy for the simulation of the other energies.

2.3.2. Simulation of the production yield using the MCNPX code The normalized distribution functions P(E) was computed from the F4 tally (proton flux) data using MCNPX code. The simulation yield was calculated as )Fassbender, et al., 2007): ( )

(

)∫

( ) ( )

( )

where A(t) is the product nuclide radioactivity, is the beam current, ρ is the target material density, d is the target thickness, L is the Avogadro constant, M is the target material molar, λ is the decay constant of the product isotope and t is the irradiation time. P(E) is the particle distribution function computed from MCNPX code and the σ(E) is the cross-section. The simulation was run with a history of 107 projectiles and the projectile flux was divided into a series of 0.5 MeV energy regions. The thickness of the target was estimated using the SRIM code. The particle distribution function P(E) was reported from the F4 tally output data that was normalized over the entire particle energy range. Default MCNPX physics model (Bertini/Dresner) for flux and distribution, was used.

3. Results and discussion 5

3.1. Calculation of excitation function The theoretical production cross-section of 89Y(p,n)89Zr is first presented. Figure 2 shows the excitation function of the 89Y(p,n)89Zr reaction for the residual nuclides from the TALYS-1.8 code. As seen, the best range of energy for this reaction is 5 to 18 MeV of proton energy. The optimum range of energy to avoid isotope and non-isotope impurities and provide a suitable production yield was 5 to 15 MeV. Figure 3 shows the cross-section of

89

Zr by

89

Y(p,n)89Zr reaction calculated using TALYS-

1.8 (HFB model) compared with the data extracted from the TENDL-2015 library (Koning, et al., 2014) and experimental data. As seen, the data extracted by TENDL-2015 library based on the TALYS code with default parameters, showed a shape that was similar to others graphs but at slightly higher magnitudes in the optimum range of energy. The results of TALYS-1.8 code showed good agreement with the experimental values for the shape and magnitude. The HFB model is closer to the data reported by Omara (Omara, et al., 2009), Khandaker (Khandaker, et al., 2012), Zhao (Zhao, et al., 1992), Sathesh (Sathesh, et al., 2011) and Mustafa (Mustafa, et al., 1988) in the optimum range of proton energy. Figure 3 shows that the peak of the cross-sections was at 13 MeV proton energy and the average of experimental cross-sections in this energy assessed 750 mb whereas this value was 815 mb and 861.6 mb

for TALYS-1.8 (HFB model) and TENDL-2015 (TALYS default)

respectively. TALYS-1.8 based on HFB model was closer to experimental so, in this work the HFB model was exerted to the calculation integral yield.

3.2. Calculation of the integral yield The theoretical integral yield of 89Zr radionuclide was obtained by measuring the production cross-section and the stopping power of

89

Y for 5-40 MeV initial proton energy as the

integral yield decreased to the threshold energy (Ethe = 3.66 MeV) for the

6

89

Y(p,n)89Zr

reaction (Equation 1). The cross-section was issued by the TALYS-1.8 code (HFB model) and the stopping power deduced from SRIM-2013 code. In particular, to estimate the

89

Zr product yield at 15 MeV protons (optimum energy),

89

Y

target was supposed irradiated for 1 h using a 1 μA proton beam current. According to the SRIM code the required target thickness for 15 MeV proton energy should be about 1 mm. The particle distribution function P(E) was reported from the F4 tally and output data normalized over the entire particle energy range (Figure 4). The cross-section deduced from the TALYS-1.8 code was used to calculate the product function P(E)σ(E). Then, the integral yield was calculated for 15 MeV proton energy using Equation 2. Likewise, the simulation integral yields was calculated for 5 to 40 MeV incident-proton energy in the same manner. Figure 5 shows the curve of integral yield for each incident-proton energy to the threshold. Finally, the results were compared with theoretical integral yield and experimental results obtained by Khandaker using the

89

Y(p,n)89Zr reaction. As seen in figure 5, there is good

agreement between the simulated integral yields and the experimental values up to 40 MeV. In the other words, there is perfect overlap up to 20 MeV of incident protons and acceptable result for 20 to 40 MeV energies. In particular, for the best-suited energy for the pointed reaction, the integral yield based on MCNPX code was 93 MBq/µA.h in comparison with the experimental results of 94.4 MBq/µA.h. (Table 1). Eventually, the integral yield was calculated for the reactions of 89Y(d,2n)89Zr, natSr(α,xn)89Zr and

nat

Zr(p,pxn)89Zr using MCNPX code using similar methods. Table 1 compares the

theoretical, simulated and experimental integral yield for different reactions of

89

Zr

production. The isotopic-impurities are also produced in specified ranges, as the separation of isotopic impurities is not possible by chemical methods. (83.4 d) impurities are generated in generated by the

89

nat

Sr(α,xn)89Zr also

90

90

Zr (stable),

91

Zr (stable) and 88Zr

Zr (stable) and

88

Zr (83.4 d) are

Y(d,2n)89Zr reaction. Most zirconium isotopes are generated by

7

nat

Zr(p,pxn)89Zr. The integral yield was simulated for the

88

Zr radionuclide, an important

impurity that features a long half-life, for the noted reactions in Table 1. In an ideal reaction, 89

Y(p,n)89Zr, the production yield of

problematic. As demonstrated, the

88

89

Zr is so insignificant (0.15 MBq/µA) that it can be

Y(p,n)89Zr reaction is the best candidate for

89

Zr

production because of its rather high specific activity and low isotopic-impurity in lowenergy cyclotrons.

3.3 General experimental details The purpose of this investigation was product Zirconium-89 by 89Y(p,n)89Zr reaction at the AMIRS (Cyclone-30, IBA, Belgium) cyclotron. To prepare the target, a certain amount of Y2O3 powder (99.99%, product of Germany) appreciate to the Al-holder dimension, was compressed into the disk-form (15 tons/cm2). The density of the disk-target assessed about 3.5 g/cm3. The pressed powder, placed in Aluminum holder then fixed by Al-cap under pressure of 30 tons/cm2 (Fig.6). The incident beam energy on target calculated using stopping power values for Yttrium Oxide and Aluminum. The target was irradiated for 1 hour by 15 MeV incident-proton energy at 20 μA beam current. During the irradiation, the target was cooled by circulating water. 15 hours after bombardment, the radionuclide purity was determined via γ-ray spectroscopy by HPGe detector (Canberra TM model GC1020-7500SL) (Figure 7). As seen in Figure 7, only 511 and 909 keV γ-rays consistence with the known spectrum of

89

Zr could be found on the γ-

energy spectrum. In this experiment the energy window was Ep = 15→10.5 MeV. The chemical separation Zirconium from yttrium was based on well-known method (Tang, et al., 2016). Dowex1X8 anion exchange resin (100-200 mesh), which was heated 90℃ with 10% NaCl and 0.2% NaOH for 2 hours has been used as resin. Deionized water was used for

8

the resin to neutralization and eluted with 0.5% HCl for 1 hour. A bout 15 hours after bombardment, the irradiated Yttrium Oxide-disk released from Al-holder and dissolved by 1 mol/L HCl then the activity of produced radioisotopes have measured through γ-ray spectroscopy by HPGe detector. To separate Yttrium from Zirconium, the target was dissolved by 10 mL of 12 mol/L HCl eluted to the resin column. In this phase of operation, Yttrium washed by 60 mL of 12 mol/L HCl. Finally, 20mL HCl 2 mol/L was used to elute Zirconium through the resin column. The solution was loaded and the γ-energy spectrum diagram reported only spectrum of Zirconium-89. In this work, the result of bombardment of Yttrium Oxide in the disk-form, was in good agreement with code calculation. Over the energy rang Ep = 15→10.5 MeV, the experimental yield of 89Zr was 53.1 MB/µA.h that is while, the simulation value predicted 57 MB/µA.h at the same energy. In figure 5, the experimental integral yield extrapolated for Ep = 15 MeV to the threshold energy and compared with the simulation at the same energy. The consistency of Monte Carlo code calculation and experimental data shows that this simulation method is very effective to estimate the integral yield to improve the status of production.

4. Conclusion In recent years, researchers have focused on

89

Zr, a radionuclide with near-ideal properties

for PET. The present study described the Monte Carlo method to investigate radionuclides using ideal reaction

89

Y(p,n)89Zr for low-energy cyclotrons. TALYS-1.8 was used to

determine the excitation function and the best range of energy. Good agreement was found in the comparison of the simulated integral yield, theoretical results, and experimental. Also, the

9

result of presented experimental work eexpresses adjustment to the simulation for the formation of

89

Zr. These results confirm that the MCNPX code can estimate the production

yield of radionuclide production with relatively high accuracy.

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Y(p, 2n)88Zr, and

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Y(p,

Y(p, pn)88Y reactions up to 40 MeV. Physical Review C,

38(4), 1624. Omara, H .M., Hassan, K. F., Kandil, S. A., Hegazy, F. E., Saleh1, Z. A., 2009. Proton induced reactions on

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Y with particular reference to the production of the medically

interesting radionuclide 89Zr. Radiochim. Acta 97, 467–471 Qaim, S.M., 2011. Cyclotron production of medical radionuclides. In: Vertis, A., Nagy, S., Klencsar, Z., Lovas, R. G., Rosch, F. (Ed.), Handbook of Nuclear Chemistry, Second edition, Springer Science, 4, pp. 1904–1930. Sadeghi, M., Aboudzadeh, M., Zali, A., Zeinali, B., 2009.

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Zr via various nuclear reactions by ALICE/ASH code. Int. J. Mod. Phys. E. 20, 1775–

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1786. Sadeghi, M., Enferadi, M., Bakhtiari, M., 2012. Accelerator production of the positron emitter zirconium-89. Ann. Nucl. Energy. 41, 97. Sadeghi, M., Jokar, N., Kakavand, T., Tenreiro, C., 2013. Prediction of

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593. Yiğit, M., Tel, E., 2015. Reaction cross-sections in the interactions of neutrons with Yttrium nucleus. J. Radioanal Nucl Chem. 306(1), 203-211. Yiğit, M., Tel, E., Sarpün, I., H., 2016. Excitation function calculations for α + 93Nb nuclear reactions. Inst. Meth. Phys. Res. B. 385, 59-64. Zhao, W., Shen Q., Lu Hanlin, Yu, W., 1992. Investigation of 89Y(p,n)89Zr,89Y(p,2n)88Zr and 12

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Ziegler, JF. 2013. Interactions of ions with matter. http://www.srim.org/. Accessed 19 Nov 2015. Zweit, J., Downey, S., Sharma, H. L., 1991. Production of no-carrier-added zirconium-89 for positron emission tomography. Appl. Radiat. Isot. 42, 199-201.

13

Table 1 Comparison between the theoretical, simulation based on MCNPX and reported experimental yield for different reactions of 89Zr production. Reaction

range

Y(p,n)89Zr

89

Y(d,2n) 89Zr

nat

nat

Sr(α,xn)89Zr

Zr(p,pxn)89Zr

⁄

)

SRIM

MCNPX

Isotopic

Experimental

Reference

Theoretical

Simulation

impurity

(This work)

(This work)

(88Zr)

15 → 4

93.32

93

0.15

94.4

Khandaker, 2012

15 → 10.5

56.6

57

53.1

This work

14 → 9

62

64

58

Omara, 2009

16 →7

57.6

56.0

66.6

Zweit, 1991

17 → 10

62.4

62.6

26 → 8.5

1.7

1.9

1.6

Kandil, 2007

40 →30

23.1

24.3

25 → 15

118.2

117.4

100.7

Uddin, 2008

(MeV)

89

Yield (

Energy

0.07

0.13

14

Fig. 1 The target geometry employed for the MCNPX input.

15

Fig. 2 Excitation function of 89Y(p, n)89Zr reaction by the TALYS-1.8 code.

16

Fig. 3 Comparison of the theoretical results of 89Zr by the TALYS-1.8 code with the reported experimental data.

17

Fig. 4 Normalized energy distribution function (MCNPX tally) for proton in the 89Y target body.

18

Fig. 5 Comparison between the theoretical integral yield, calculation based on MCNPX and reported experimental data using 89Y(p,n)89Zr reaction.

19

Fig. 6 Yttrium oxide in the Al-holder (before bombardment).

20

Fig. 7 The γ-energy spectrum diagram of Zirconium solution.

Highlights 1. An experimental yield of 51.3 MB/µA·h was obtained for the 15 MeV proton-induced on Y2O3. 2. The formation of 89Zr was simulated using the Monte Carlo simulation code. 3. Good agreement was found in the simulated and experimental integral yield.

21