用于医用核素钼-99的制备方法
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摘要
~(99)Mo的衰变子体核素~(99m)Tc是核医学中应用最为广泛的放射性同位素,其使用量约占所有放射性同位素的70%。基于对目前国内外~(99)Mo制备方法的文献调研,阐述了医用~(99)Mo的主要制备方法,包括反应堆生产~(99)Mo、加速器制备~(99)Mo和中子发生器制备~(99)Mo。从靶件形式与化学提取等方面重点分析了以高浓铀(HEU)或低浓铀(LEU)为靶材料,利用反应堆生产裂变~(99)Mo的方法。鉴于近年来使用加速器与中子发生器制备~(99)Mo的方法已取得了较大进展,本文亦对此进行了较详细的阐述,并对进一步的研究工作提出建议。
~(99m)Tc,as the decay daughter of ~(99)Mo,is the most frequently used radionuclide in nuclear medicine. The usage of ~(99)Mo is not less than 70% of that of the all radioisotopes. The methods for ~(99)Mo production by nuclear reactors,accelerators and neutron generators were studied. Here,based on the investigated literatures,methods for ~(99)Mo production had been analyzed with an emphasis on ~(99)Mo production extracted from235 U fission products with high enriched uranium( HEU) or low enriched uranium( LEU) target. Due to the recently rapid development of methods for ~(99)Mo production by accelerators and neutron generators,the achieved progresses were reviewed in this respect. In the present paper,some advices were also given for further exploration.
~(99m)Tc,as the decay daughter of ~(99)Mo,is the most frequently used radionuclide in nuclear medicine. The usage of ~(99)Mo is not less than 70% of that of the all radioisotopes. The methods for ~(99)Mo production by nuclear reactors,accelerators and neutron generators were studied. Here,based on the investigated literatures,methods for ~(99)Mo production had been analyzed with an emphasis on ~(99)Mo production extracted from235 U fission products with high enriched uranium( HEU) or low enriched uranium( LEU) target. Due to the recently rapid development of methods for ~(99)Mo production by accelerators and neutron generators,the achieved progresses were reviewed in this respect. In the present paper,some advices were also given for further exploration.
引文
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[39]Rao A,Sharma A K,Kumar P,et al.Studies on separation and purification of fission99Mo from neutron activated uranium aluminum alloy[J].Applied Radiation and Isotopes,2014,89:186-191.
[40]王清贵,梁积新,吴宇轩,等.α-安息香肟沉淀法分离低浓铀裂变产物中的钼[J].同位素,2016,29(3):216-222.Wang Qinggui,Liang Jixin,Wu Yuxuan et al,Separation of fission molybdenum from low enriched uranium products by precipitation withα-Benzoin Oxime[J].Journal of Isotopes,2016,29(3):216-222(in Chinese).
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[42]Chung C,Woo M Y.Fission product yields in the fast-neutron fission of238U[J].Journal of Radioanalytical and Nuclear Chemistry,1987,109(1):117-131.
[43]Naik H,Nair A G C,Kalsi P C,et al.Absolute fission yields in the fast neutron induced fission of99.9997 atom%pure238U using track￡tch-cum gamma spectrometric technique[J].Radiochimica Acta,1996,75(2):69-76.
[44]Naik H,Suryanarayana S V,Jagadeesan K C,et al.An alternative route for the preparation of the medical isotope99Mo from the238U(γ,f)and100Mo(γ,n)reactions[J].Journal of Radioanalytical and Nuclear Chemistry,2013,295(1):807-816.
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[46]Pupillo G,Esposito J,Haddad F,et al.Accelerator-based production of99Mo:a comparison between the100Mo(p,x)and96Zr(α,n)reactions[J].Journal of Radioanalytical and Nuclear Chemistry,2015,305(1):73-78.
[47]Kudo H,Muramatsu H,Nakahara H,et al.Fission fragmentyields in the fission of232Th by proton of energies 8 to 22 Me V[J].Physical Review C,1982,25:3 011-3 023.
[48]Demetriou P,Keutgen T,Prieels R,et al.Fission properties of actinide nuclei from proton-induced fission at 26.5 and 62.9 Me V incident proton energies[J].Physical Review C,2010,82:054606-1-054606-11.
[49]Abbas K,Holzwarth U,Simonelli F,et al.Feasibility of99Mo production by proton-induced fission of232Th[J].Nuclear Instruments and Methods in Physics Research B,2012,278:20-25.
[50]Mirvakili S M,Alizadeh M,Vaziri J A,et al.Computational investigation of99Mo production yield via proton irradiation ofnatU and232Th targets[J].Applied Radiation and Isotopes,2015,101:127-134.
[51]Lebeda O,Fikrle M.New measurement of excitation functions for(d,x)reactions onnatMo with special regard to the formation of95mTc,96m+gTc,99mTc and99Mo[J].Applied Radiation and Isotopes,2010,68:2 425-2 432.
[52]Pupillo G,Esposito J,Gambaccini M,et al.Experimental cross section evaluation for innovative99Mo production via the(a,n)reaction on96Zr target[J].Journal of Radioanalytical and Nuclear Chemistry,2014,302:911-917.
[53]Ruth T.Accelerating production of medical isotopes[J].Nature,2009,457:29.
[54]Naik H,Nimje V T,Raj D,et al.Mass distribution in the bremsstrahlung-induced fission of232Th,238U and240Pu[J].Nuclear Physics A,2011,853:1-25.
[55]Nagai Y,Hatsukawa Y.Production of99Mo for nuclear medicine by100Mo(n,2n)99Mo[J].Journal of the Physical Society of Japan,2009,78(3):033201-1-033201-4.
[56]National Nuclear Data Center[EB/OL].http:∥www.nndc.bnl.gov/.
[57]Fadil M,Rannou B.The SPIRAL2 project team[J].Nuclear Instruments and Methods in Physics Research Section B,2008,266:4 318.
[58]Nagai Y.99Mo Production via100Mo(n,2n)99Mo using accelerator neutrons[J].EPJ Web of Conferences,2014,66:10 007.
[59]Stevenson N R,Schenter R E.Molybdenum-99production with high specificactivity using medium energy neutrons on technetium or ruthenium targets[J].Journal of Labelled Compounds and Radiopharmaceuticals,2010,53:332-345.
[2]National Academies of Sciences,Engineering,and Medicine.Molybdenum-99 for medical imaging[M].Washington:The National Academies Press,2016:58.
[3]World Nuclear Association.Radioisotopes in medicine[J/OL].Accessed from http:∥www.worldnuclear.org/information-library/non-power-nuclearapplications/radioisotopes-research/radioisotopes-inmedicine.aspx,December 2017.
[4]National Research Council.Medical isotope production without highly enriched uranium[M].Washington:The National Academies Press,2009:3.16-3.18.
[5]Ponsard B.Mo-99 supply issues:Status report and lessons learned[C]∥14th International Topical Meeting on Research Reactor Fuel Management(RRFM 2010).Berne:European Nuclear Society,2010.
[6]Ball R M.Characteristics of nuclear reactors used for the production of molybdenum-99[R].Vienna:International Atomic Energy Agency,1999,IAEATECDOC-1 065:5-17.
[7]Ball R M,Pavshook V A,Khvostionovv V Y.Present status of the use of LEU in aqueous reactors to produce Mo-99,reduced enrichment for research and test reactors[C]∥1998 International Meeting on Reduced Enrichment for Research and Test Reactors.Sao Paulo:October 18,1998.
[8]Stepinski D C,Gelis A V,Gentner P,et al.Evaluation of radsorb,isosorb(termoxid)and PZC as potential sorbents for separation of99Mo from a homogeneous-reactor fuel solution[R].Vienna:International Atomic Energy Agency,2008,IAEATECDOC-1601:73-80.
[9]Chuvilin D Y,Khvostionov V E,Markovskij D V,et al.Low-waste and proliferation-free production of medical radioisotopes in solution and molten-salt reactors[M]∥Radioactive waste.Rijeka:In Tech,2012:153-156.
[10]Chuvilin D Y,Meister J D,Abalin S S,et al.An interleaved approach to production of99Mo and89Sr medical radioisotopes[J].J Radioanal Nucl Chem,2003,257(1):59-63.
[11]Pavshook V A.Effective method of99Mo and89Sr production using liquid fuel reactor[R].Vienna:International Atomic Energy Agency,2008,IAEATECDOC-1 601:65-68.
[12]Inaba Y.Development of99Mo production technology with solution irradiation method[M]∥Nuclear reactors.Rijeka:In Tech,2012:324-325.
[13]Tucker W D,Greene M W,Weiss A J,et al.Methods of preparation of some carrier-free radioisotopes involving sorption on alumina[R].NY:Brookhaven National Lab,Upton,1958.
[14]Arino H,Cosolito F J,George K D,et al.Preparation of a primary target for the production of fission products in a nuclear reactor:US,3,940,318[P].1976-02-24.
[15]Arino H,Thornton A,Kramer H.Production of high purity fission product molybdenum-99:U S,3,799,883[P].1974-03-26.
[16]Technical Reports Series No.478,Feasibility of producing molybdenum-99 on a small scale using fission of low enriched uranium or neutron activation of natural molybdenum[R].VIENNA:IAEA,2014:64-66.
[17]Lee S K,Beyer G J,Lee J S.Development of industrial-scale fission99Mo production process using low enriched uranium target[J].Nuclear Engineering and Technology,2016,48(3):613-623.
[18]National Research Council.Medical isotope production without highly enriched uranium[C]∥Committee on medical isotope production without highly enriched uranium.Washington:The National Academies Press,2009:2.1-2.13.
[19]Vandegrift G F,Snelgrove J L,Aase S,et al.Converting targets and processes for fission-product molybdenum-99 from high-to low-enriched uranium[R].Vienna:International Atomic Energy Agency,1999,IAEA-TECDOC-1 065:28.
[20]Salacz J.Production of fission Mo-99,I-131 and Xe-133[J].Revue IRE Tijdschrift,1985,9(3):22.
[21]Van der Walt T N,Coetzee P P.The isolation of99Mo from fission material for use in the99Mo/99mTc generator for medical use[J].Radiochimica Acta,2004,92(4-6):251-257.
[22]缪增星,马会民,刘建民,等.医用裂变99Mo的生产工艺研究[J].中国原子能科学研究院年报,1989,0:146-147.Miu Zengxing,Ma Huimin,Liu Jianmin,et al.Study on the production process of medical fission99Mo[J].Annual Report of China Institute of Atomic Energy,1989,0:146-147(in Chinese).
[23]缪增星,马会民,刘建民,等.裂变99Mo生产工艺研究的进展[J].中国原子能科学研究院年报,1990,1:162-163.Miu Zengxing,Ma Huimin,Liu Jianmin,et al.Progress in the production process of fission99Mo[J].Annual Report of China Institute of Atomic Energy,1990,1:162-163(in Chinese).
[24]肖伦.放射性同位素技术[M].北京:原子能出版社,2000:43-45.
[25]Sameh A,Ache H J.Production techniques of fission molybdenum-99[J].Radiochimica Acta,1987,41(2-3):65-72.
[26]Sameh A A,Ache H J.Production techniques of fission99Mo[R].Vienna:International Atomic Energy Agency,1989,IAEA-TECDOC-515:47-64.
[27]Chuvilin D Y,Khvostionov V E,Markovskij D V,et al.Production of89Sr in solution reactor[J].Applied Radiation and Isotopes,2007,65(10):1087-1 094.
[28]Ponomarev-Stepnoy N N,Pavshook V A,Bebikh G F,et al.Method and apparatus for the production and extraction of molybdenum-99:U S,5,910,971[P].1999-06-08.
[29]Betenekov N D,Denisov E I,Nedobukh T A,et al.Inorganic sorbent for molybdenum-99 extraction from irradiated uranium solutions and its method of use:U S,6,337,055[P].2002-01-08.
[30]邓启民,李茂良,程作用.医用同位素生产堆(MIPR)生产99Mo的应用前景[J].核科学与工程,2006,26(2):165-167.Deng Qimin,Li Maoliang,Cheng Zuoyong.Application of99Mo production through Medical Isotope Production Reactor(MIPR)[J].Chinese Journal of Nuclear Science and Engineering,2006,26(2):165-167(in Chinese).
[31]National Research Council.Medical isotope production without highly enriched uranium[C].Washington:The National Academies Press,2009:7.1-7.2.
[32]Novotny D,Wagner G.Procedure of small scale production of Mo-99 on the basis of irradiated natural uranium metal as target[C]∥Proceedings of the Consultants Meeting on“Small Scale Production of fission Mo-99 for Use in Tc-99m Generators.Vienna:International Atomic Energy Agency,2003.
[33]Dittrich S.History and actual state of non-HEU fission-based Mo-99 production with low-performance research reactors[J].Science and Technology of Nuclear Installations,2013:4.
[34]Snelgrove J L,Hofman G L,Wiencek T C,et al.Development and processing of LEU targets for99Mo production—Overview of the ANL Program[C]∥the 1995 International Meeting.Paris:Reduced Enrichment for Research and Test Reactors.Vienna:International Atomic Energy Agency,1995:18-21.
[35]Conner C,Sedlet J,Wiencek T C,et al.Production of MO-99 from LEU targets acid-side processing[R].IL(US):Argonne National Lab,2000:5-9.
[36]Vandegrift G F,Conner C,Hofman G L,et al.Modification of targets and processes for conversion of99Mo production from high-to low-enriched uranium[J].Industrial&engineering chemistry research,2000,39(9):3 140-3 145.
[37]Mushtaq A,Iqbal M,Muhammad A.Management of radioactive waste from molybdenum-99 production using low enriched uranium foil target and modified CINTICHEM process[J].Journal of Radioanalytical and Nuclear Chemistry,2009,281(3):379-392.
[38]Vandegrift G F,Koma Y,Cols H,et al.Production of MO-99 from LEU targets base-side processing[R].IL(US):Argonne National Lab,2000:3-6.
[39]Rao A,Sharma A K,Kumar P,et al.Studies on separation and purification of fission99Mo from neutron activated uranium aluminum alloy[J].Applied Radiation and Isotopes,2014,89:186-191.
[40]王清贵,梁积新,吴宇轩,等.α-安息香肟沉淀法分离低浓铀裂变产物中的钼[J].同位素,2016,29(3):216-222.Wang Qinggui,Liang Jixin,Wu Yuxuan et al,Separation of fission molybdenum from low enriched uranium products by precipitation withα-Benzoin Oxime[J].Journal of Isotopes,2016,29(3):216-222(in Chinese).
[41]Le V S.99mTc generator development:Up-to-date99mTc-recovery technologies for increasing the effectiveness of99Mo utilization[J].Sci.Technol Nucl Install,2014.
[42]Chung C,Woo M Y.Fission product yields in the fast-neutron fission of238U[J].Journal of Radioanalytical and Nuclear Chemistry,1987,109(1):117-131.
[43]Naik H,Nair A G C,Kalsi P C,et al.Absolute fission yields in the fast neutron induced fission of99.9997 atom%pure238U using track￡tch-cum gamma spectrometric technique[J].Radiochimica Acta,1996,75(2):69-76.
[44]Naik H,Suryanarayana S V,Jagadeesan K C,et al.An alternative route for the preparation of the medical isotope99Mo from the238U(γ,f)and100Mo(γ,n)reactions[J].Journal of Radioanalytical and Nuclear Chemistry,2013,295(1):807-816.
[45]Qaim S M,Sudár S,Scholten B,et al.Evaluation of excitation functions of100Mo(p,d+pn)99Mo and100Mo(p,2n)99mTc reactions:estimation of longlived Tc-impurity and its implication on the specific activity of cyclotron-produced99mTc[J].Applied Radiation and Isotopes,2014,85:101-113.
[46]Pupillo G,Esposito J,Haddad F,et al.Accelerator-based production of99Mo:a comparison between the100Mo(p,x)and96Zr(α,n)reactions[J].Journal of Radioanalytical and Nuclear Chemistry,2015,305(1):73-78.
[47]Kudo H,Muramatsu H,Nakahara H,et al.Fission fragmentyields in the fission of232Th by proton of energies 8 to 22 Me V[J].Physical Review C,1982,25:3 011-3 023.
[48]Demetriou P,Keutgen T,Prieels R,et al.Fission properties of actinide nuclei from proton-induced fission at 26.5 and 62.9 Me V incident proton energies[J].Physical Review C,2010,82:054606-1-054606-11.
[49]Abbas K,Holzwarth U,Simonelli F,et al.Feasibility of99Mo production by proton-induced fission of232Th[J].Nuclear Instruments and Methods in Physics Research B,2012,278:20-25.
[50]Mirvakili S M,Alizadeh M,Vaziri J A,et al.Computational investigation of99Mo production yield via proton irradiation ofnatU and232Th targets[J].Applied Radiation and Isotopes,2015,101:127-134.
[51]Lebeda O,Fikrle M.New measurement of excitation functions for(d,x)reactions onnatMo with special regard to the formation of95mTc,96m+gTc,99mTc and99Mo[J].Applied Radiation and Isotopes,2010,68:2 425-2 432.
[52]Pupillo G,Esposito J,Gambaccini M,et al.Experimental cross section evaluation for innovative99Mo production via the(a,n)reaction on96Zr target[J].Journal of Radioanalytical and Nuclear Chemistry,2014,302:911-917.
[53]Ruth T.Accelerating production of medical isotopes[J].Nature,2009,457:29.
[54]Naik H,Nimje V T,Raj D,et al.Mass distribution in the bremsstrahlung-induced fission of232Th,238U and240Pu[J].Nuclear Physics A,2011,853:1-25.
[55]Nagai Y,Hatsukawa Y.Production of99Mo for nuclear medicine by100Mo(n,2n)99Mo[J].Journal of the Physical Society of Japan,2009,78(3):033201-1-033201-4.
[56]National Nuclear Data Center[EB/OL].http:∥www.nndc.bnl.gov/.
[57]Fadil M,Rannou B.The SPIRAL2 project team[J].Nuclear Instruments and Methods in Physics Research Section B,2008,266:4 318.
[58]Nagai Y.99Mo Production via100Mo(n,2n)99Mo using accelerator neutrons[J].EPJ Web of Conferences,2014,66:10 007.
[59]Stevenson N R,Schenter R E.Molybdenum-99production with high specificactivity using medium energy neutrons on technetium or ruthenium targets[J].Journal of Labelled Compounds and Radiopharmaceuticals,2010,53:332-345.