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Accurate determination of production data of the non-standard positron emitter 86Y via the 86Sr(p,n)-reaction

  • M. Shuza Uddin , Bernhard Scholten , M. Shamsuzzhoha Basunia , Sandor Sudár , Stefan Spellerberg , Andrew S. Voyles , Jonathan T. Morrell , Haleema Zaneb , Jesus A. Rios , Ingo Spahn , Lee A. Bernstein , Bernd Neumaier and Syed M. Qaim EMAIL logo
Published/Copyright: July 13, 2020
Radiochimica Acta
From the journal Radiochimica Acta Volume 108 Issue 9

Abstract

In view of several significant discrepancies in the excitation function of the 86Sr(p,n)86g+xmY reaction which is the method of choice for the production of the non-standard positron emitter 86Y for theranostic application, we carried out a careful measurement of the cross sections of this reaction from its threshold up to 16.2 MeV at Forschungszentrum Jülich (FZJ) and from 14.3 to 24.5 MeV at LBNL. Thin samples of 96.4% enriched 86SrCO3 were prepared by sedimentation and, after irradiation with protons in a stacked-form, the induced radioactivity was measured by high-resolution γ-ray spectrometry. The projectile flux was determined by using the monitor reactions natCu(p,xn)62,63,65Zn and natTi(p,x)48V, and the calculated proton energy for each sample was verified by considering the ratios of two reaction products of different thresholds. The experimental cross section data obtained agreed well with the results of a nuclear model calculation based on the code TALYS. From the cross section data, the integral yield of 86Y was calculated. Over the optimum production energy range Ep = 14 → 7 MeV the yield of 86Y amounts to 291 MBq/μA for 1 h irradiation time. This value is appreciably lower than the previous literature values calculated from measured and evaluated excitation functions. It is, however, more compatible with the experimental yields of 86Y obtained in clinical scale production runs. The levels of the isotopic impurities 87mY, 87gY, and 88Y were also estimated and found to be <2% in sum.

Keywords: cross section; excitation function; integral yield and isotopic purity of the product; nuclear model calculation; proton irradiation; 86SrCO3 thin sample
Corresponding author: Syed M. Qaim, Institut für Neurowissenschaften und Medizin, INM-5: Nuklearchemie, Forschungszentrum Jülich, 52425Jülich, Germany, E-mail:

Funding source: Lawrence Berkeley National Laboratory

Funding source: University of South Alabama

Acknowledgments

M. S. Uddin thanks the Alexander von Humboldt (AvH) Foundation in Germany and Lawrence Berkeley National Laboratory, USA, for financial support. He would also like to acknowledge the authorities of Bangladesh Atomic Energy Commission and Ministry of Science and Technology, Dhaka, Bangladesh, for granting leave of absence to conduct these experiments abroad. H. Zaneb thanks the LBNL and the Higher Education Commission (HEC) of Pakistan for the opportunity and support to conduct a piece of research abroad while doing her Ph.D. work at the Physics Department of Government College University Lahore, Pakistan. We all thank the operation crews of the cyclotron BC1710 at FZJ and 88-inch cyclotron at LBNL for their help in irradiation of samples. The work at LBNL was performed under the auspices of the U.S. Department of Energy under contract No. DE-AC02-05CH11231. This research is supported by the U.S. Department of Energy Isotope Program, managed by the Office of Science for Nuclear Physics.

  1. Author contribution: All the authors have accepted responsibility for the entire content of this submitted manuscript and approved submission.

  2. Research funding: M. S. Uddin thanks the Alexander von Humboldt (AvH) Foundation in Germany and Lawrence Berkeley National Laboratory, USA, for financial support.

  3. Conflict of interest statement: The authors declare no conflicts of interest regarding this article.

Appendix Formation cross sections and integral yields of the isotopic impurities 87mY, 87gY and 88Y

During the measurements on the 86Sr(p,n)86g+xmY reaction described above, cross sections of three subsidiary reactions, namely 87Sr(p,n)87mY, 87Sr(p,n)87gY and 88Sr(p,n)88Y, leading to the isotopic impurities 87mY, 87gY and 88Y, respectively, were also measured. The data obtained for only 1.33% abundant 87Sr and 2.26% abundant 88Sr in the enriched 86Sr were extrapolated to 100% abundance each, and the results are given in Appendix Table 1. The extrapolation of results for the 88Sr(p,n)88Y reaction was straightforward because no other reaction contributes to the formation of 88Y. In the case of the 87Sr(p,n)87mY and 87Sr(p,n)87gY reactions, however, extrapolation was appropriate only up to 14 MeV. Beyond that energy range, corrections for the contributions of the 88Sr(p,2n)87m,gY processes were necessary. We applied those corrections by using the evaluated data reported by Zaneb et al. [7]. The extrapolated data for 88Y agreed with the results of two previous careful measurements [10], [24] in which natSrCO3 samples (with 88Sr abundance of 82.58%) were used as targets. This added confidence to our present measurement.

For constructing the excitation function of the 88Sr(p,n)88Y reaction, we adopted the basic diagram by Zaneb et al. [7] and added the new data [24 and this work] to it. A polynomial function was then fitted to all the concordant points and the curve thus obtained was used for the yield calculation. For the 87Sr(p,n)87mY reaction, three sets of data exist in the literature [10], [24], [26]. Our data agree very well with the values by Kettern et al. [10] and Elbinawi et al. [24] but not with Levkovskii [26] (cf. Appendix Figure 1). A polynomial fit through the three concordant datasets [10], [24], and [this work] gave the required curve for the yield calculation. The data for the 87Sr(p,n)87gY reaction are shown in Appendix Figure 2. They describe the independent formation of 87gY, i. e., without any contribution from the decay of 87mY. In this case a polynomial fit through own data points was carried out.

From the fitted excitation functions of the above mentioned three reactions, the integral yields of 87mY, 87gY and 88Y were calculated for 100% abundance of the target isotope, assuming a 1 h irradiation with a proton beam current of 1 μA. The result is given in Appendix Figure 3. Those data should allow calculation of the three radionuclidic impurities under consideration while using an enriched 86Sr target of any isotopic composition.

Appendix Figure 1: Excitation function of the 87Sr(p,n)87mY reaction.
Appendix Figure 1:

Excitation function of the 87Sr(p,n)87mY reaction.

Appendix Figure 2: Excitation function of the 87Sr(p,n)87gY reaction. The data describe the independent formation cross sections of 87gY.
Appendix Figure 2:

Excitation function of the 87Sr(p,n)87gY reaction. The data describe the independent formation cross sections of 87gY.

Appendix Figure 3: Integral yields of the radionuclides 87mY, 87gY and 88Y, calculated from the measured excitation functions of the 87Sr(p,n)87mY, 87Sr(p,n)87gY and 88Sr(p,n)88Y processes, assuming 100% abundance of the target isotope and an irradiation time of 1 h. The curves are shown as a function of the proton energy.
Appendix Figure 3:

Integral yields of the radionuclides 87mY, 87gY and 88Y, calculated from the measured excitation functions of the 87Sr(p,n)87mY, 87Sr(p,n)87gY and 88Sr(p,n)88Y processes, assuming 100% abundance of the target isotope and an irradiation time of 1 h. The curves are shown as a function of the proton energy.

Appendix Table 1:

Cross sections for the formation of isotopic impurities 87mY, 87gY and 88Y.

Proton energy (MeV)CyclotronMeasured cross sections (mb)
87Sr(p,n)87mY87Sr(p,n)87gYa88Sr(p,n)88Y
24.5 ± 0.488-inch12 ± 1.620 ± 347 ± 7
22.5 ± 0.415 ± 226 ± 451 ± 7
20.5 ± 0.444 ± 624 ± 396 ± 14
18.4 ± 0.585 ± 1257 ± 8221 ± 31
17.0 ± 0.5165 ± 2385 ± 12376 ± 53
15.7 ± 0.5296 ± 41144 ± 20606 ± 86
14.3 ± 0.5433 ± 56168 ± 24656 ± 86
16.2 ± 0.2BC1710225 ± 32147 ± 21472 ± 62
16.0 ± 0.2203 ± 28133 ± 19456 ± 60
14.7 ± 0.2368 ± 52182 ± 26716 ± 94
14.3 ± 0.2394 ± 51178 ± 25720 ± 94
13.4 ± 0.3436 ± 57186 ± 26859 ± 113
13.0 ± 0.3382 ± 50190 ± 27884 ± 116
12.0 ± 0.3435 ± 57181 ± 25835 ± 110
11.0 ± 0.3457 ± 59157 ± 22753 ± 99
10.5 ± 0.3362 ± 47158 ± 22657 ± 86
9.6 ± 0.4348 ± 45132 ± 18605 ± 79
8.8 ± 0.4336 ± 44104 ± 15505 ± 66
8.3 ± 0.4316 ± 41109 ± 15456 ± 60
7.9 ± 0.4302 ± 3998 ± 14404 ± 53
6.9 ± 0.4243 ± 3287 ± 12249 ± 33
6.5 ± 0.4162 ± 2167 ± 9169 ± 22

  1. aThese cross sections are for independent formation of 87gY, i. e., without the contribution via the decay of 87mY.

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Received: 2020-03-16
Accepted: 2020-05-03
Published Online: 2020-07-13
Published in Print: 2020-09-25

© 2020 Walter de Gruyter GmbH, Berlin/Boston

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  1. Frontmatter
  2. Original Papers
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https://doi.org/10.1515/ract-2020-0021
Keywords for this article
cross section; excitation function; integral yield and isotopic purity of the product; nuclear model calculation; proton irradiation; 86SrCO3 thin sample

Articles in the same Issue

  1. Frontmatter
  2. Original Papers
  3. Measurement of 14.54 MeV neutron induced reaction cross sections of Cr and Mn with covariance analysis
  4. Simultaneous separation of Am and Cm from Nd and Sm by multi-step extraction using the TODGA-DTPA-BA-HNO3 system
  5. Influence of plutonyl ion on electrochemical characterization of zirconium in plutonium nitrate solutions
  6. Neptunium extraction by N,N-dialkylamides
  7. Ultrafast and highly capture of U(VI) by hierarchical mesoporous carbon
  8. Modification of perlite to prepare low cost zeolite as adsorbent material for removal of 144Ce and 152+154Eu from aqueous solution
  9. Production of Cf-252 and other transplutonium isotopes at Oak Ridge National Laboratory
  10. Rapid Communication
  11. Accurate determination of production data of the non-standard positron emitter 86Y via the 86Sr(p,n)-reaction
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