Synthesis and Characterization of Molybdenum Phthalocyanine as Target Material for High Specific Activity Molybdenum-99 Production

https://doi.org/10.22146/ijc.33218

Muhamad Basit Febrian(1*), Duyeh Setiawan(2), Hilda Hidayati(3)

(1) Center for Applied Science and Nuclear Technology, National Nuclear Energy Agency, Jl. Tamansari No. 71, Bandung 40132, West Java, Indonesia
(2) Center for Applied Science and Nuclear Technology, National Nuclear Energy Agency, Jl. Tamansari No. 71, Bandung 40132, West Java, Indonesia
(3) Department of Chemical Engineering, Politeknik Negeri Bandung, Jl. Gegerkalong Hilir, Ds. Ciwaruga, Bandung 40559, West Java, Indonesia
(*) Corresponding Author

Abstract


High specific activity is a necessity in the fabrication of 99Mo/99mTc radioisotope generators. Recoil reaction, or the Szilard-Chalmers effect, is a method that could be used as an alternative method for increasing specific activity in radioisotope production in light of tightening regulation of highly enriched uranium (HEU) irradiation. Phthalocyanine compounds are usually used as the target material in recoil reactions for the production of high specific radioisotope activity via the (n,γ) reaction. Molybdenum phthalocyanine (Mo-Pc) could be a promising target material in recoil reactions for producing high specific activity of 99Mo. Mo-Pc was synthesized via solid-state reaction between ammonium heptamolybdate and phthalonitrile in a reflux system at 300 °C for 3 h. This optimum condition was identified after performing several variations of temperature and time of reaction, considering FTIR spectra, the yield of product and melting point of the product. XRD measurement showed that Mo-Pc synthesized at optimum condition was free from MoO2, phthalimide and unreacted molybdenum. Mo-Pc has UV-vis properties of Q-band absorption between 600 and 750 nm when dissolved in tetrahydrofuran, dimethylformamide and trifluoroacetic acid. Splitting at absorption peak in tetrahydrofuran and dimethylformamide solution indicated that protonation had occurred. This split peak did not appear in a trifluoroacetic acid solution. In the preliminary study of irradiation of 1 g Mo-Pc at 3.5x1012 n cm–2 s–1 neutron flux, followed by dissolution in tetrahydrofuran and extraction of Mo-99 into NaOH, we obtained Mo-99 solution with a specific activity of 682.35 mCi/g Mo, this being 254.61 times higher than in the regular MoO3 target.


Keywords


recoil; high specific activity; phthalocyanine; characterization

Full Text:

Full Text PDF


References

[1] Pillai, M.R.A., Dash, A., and Knapp, F.F.R., 2013, Sustained availability of 99mTc: Possible paths forward, J. Nucl. Med., 54 (2), 313–23.

[2] IAEA, 2013, Non-HEU Production Technologies for Molybdenum-99 and Technetium-99m, 1st ed., International Atomic Energy Agency, Vienna, Austria.

[3] Le, V.S., 2014, 99mTc generator development: Up-to-date 99mTc-recovery technologies for increasing the effectiveness of 99Mo utilization, Sci Technol Nucl. Ins., 2014, 345252.

[4] Dash, A., Knapp, F.F.R., and Pillai, M.R., 2013, 99Mo/99mTc separation: An assessment of technology options, Nucl. Med. Biol., 40 (2), 167–176.

[5] Kadarisman, and Adang, H.G., 2011, Unjuk kerja generator radioisotop 99Mo/99mTc dengan radioaktivitas 99Mo 600 dan 800 mCi berbasis PZC, Urania, 17 (1), 26–33.

[6] Dikiy, N.P., Dovbnya, A.N., Krasnoslsky, N.V., Lyashko, Y.V., Medvedeva, E.P., Medvedev, D.V., Uvarov, V.L., and Fedorets, I.D., 2015, The use of molybdenum oxide nanoparticles for production of free isotope Mo-99, Probl. Atomic Sci. Technol., 100 (6), 154–156.

[7] de Crowley, L.A.F., Lara, R.O., Millan, S.S., and Maddock, A.G., 1979, Recoil effects in some molybdenum complexes, Radiochim. Acta, 26, 39–40.

[8] Ilyin, A.P., Korovin, S.A., Menshikov, L.I., Petrunin, V.F., Semenov, A.N., and Chuvilin, D.Y., 2015, Usage of molybdenum nanocrystalline powder for radioisotope production, Physics Procedia, 72, 548–551.

[9] Setiawan, D., 2000, Synthesis and Characterization of Tungsten-Phtalocyanine as Target Material of High Specific Activity W-188, Proceeding of Scientific Meeting in Radiation and Isotopes Technology Development, 269–273.

[10] Edmondson, S.J., and Mitchell, P.C.H., 1986, Molybdenum phthalocyanine, Polyhedron, 5 (1-2), 315–317.

[11] Nampira, Y., and Anggraini, D., 2012, Penggunaan pereaksi xylenol orange dalam analisis molybdenum menggunakan metode spektrophotometri, Urania, 18 (2), 88–95.

[12] Ghani, F., Kristen, J., and Riegler, H., 2012, Solubility properties of unsubstituted metal phthalocyanines in different types of solvents, J. Chem. Eng. Data, 57 (2), 439–449.

[13] Achar, B.N., Fohlen, G.M., Lokesh, K.S., and Kumar, T.M.M., 2005, GC–MS studies on degradation of copper phthalocyanine sheet polymer, Int. J. Mass Spectrom., 243 (3), 199–204.

[14] Naouel, R., Touati, F., and Gharbi, N., 2012, Control of the morphology of molybdenum dioxide nanoparticles, E-J. Chem., 9 (1), 233–239.

[15] Sarno, M., Garamella, A., Cirillo, C., and Ciambelli, P., 2014, MoO2 synthesis for LIBs, Chem. Eng. Trans., 41, 307–312.

[16] Ravisubramanian, S., Azad, A., and Sakthinathan, G., 2013, Coating of synthesized molybdenum nanopowder on aluminium, Asian J. Sci. Res., 6 (3), 603–608.

[17] Chen, X., Shan, S., Liu, J., Qu, X., and Zhang, Q., 2015, Synthesis and properties of high temperature phthalonitrile polymers based on o, m, p-dihydroxybenzene isomers, RSC Adv., 5 (98), 80749–80755.

[18] Tuhl, A., Manaa, H., Makhseed, S., Al-Awadi, N., Mathew, J., Ibrahim, H.M., Nyokong, T., and Behbehani, H., 2012, Reverse saturation absorption spectra and optical limiting properties of chlorinated tetrasubstituted phthalocyanines containing different metals, Opt. Mater., 34 (11), 1869–1877.

[19] Roth, F., Herzig, M., Lupulescu, C., Darlatt, E., Gottwald, A., Knupfer, M., and Eberhardt, W., 2015, Electronic properties of Mn-Phthalocyanine-C60 bulk heterojunctions: Combining photoemission and electron energy-loss spectroscopy, J. Appl. Phys., 118 (18), 185310.

[20] Glaser, M., Peisert, H., Adler, H., Polek, M., Uihlein, J., Nagel, P., Merz, M., Schuppler, S., and Chasse, T., 2015, Transition-metal phthalocyanines on transition-metal oxides: Iron and cobalt phthalocyanine on epitaxial MnO and TiOx films, J. Phys. Chem. C, 119 (49), 27569–27579.

[21] van Dorp, J.W.J., Mahes, D.S., Bode, P., Wolterbeek, H.T., Denkova, A.G., and Serra-Crespo, P., 2018, Towards the production of carrier-free 99Mo by neutron activation of 98Mo in molybdenum hexacarbonyl-Szilard-Chalmers enrichment, Appl. Radiat. Isot., 140, 138–145.

[22] Tomar, B.S., Steinebach, O.M., Terpstra, B.E., Bode, P., and Wolterbeek, H.T., 2010, Studies on production of high specific activity 99Mo and 90Y by Szilard Chalmers reaction, Radiochim. Acta, 98, 499–506.

[23] Febrian, M.B., Mulyati, T.S., Suherman, A., Adventini, N., Setiadi, Y., Setiawan, D., and Aziz, A., 2018, Spectrophotometric determination of molybdenum content in 99mTc solution via Mo-TGA-KSCN complexes formation, JSTNI, 19 (2), 71–80.



DOI: https://doi.org/10.22146/ijc.33218

Article Metrics

Abstract views : 3971 | views : 3347


Copyright (c) 2019 Indonesian Journal of Chemistry

Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

 


Indonesian Journal of Chemistry (ISSN 1411-9420 /e-ISSN 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.

Web
Analytics View The Statistics of Indones. J. Chem.