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Production of High-Purity Radium-223 from Legacy Actinium-Beryllium Neutron Sources†

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Production of High-Purity Radium-223 from Legacy Actinium-Beryllium Neutron Sources† 244 Current Radiopharmaceuticals, 2012, 5, 244-252 Production of High-purity Radium-223 from Legacy Actinium-Beryllium † Neutron Sources Chuck Z. Soderquist, Bruce K. McNamara and Darrell R. Fisher* Isotope Sciences Program, Pacific Northwest National Laboratory, Richland, Washington, USA Abstract: Radium-223 is a short-lived alpha-particle-emitting radionuclide with potential applications in cancer treat- ment. Research to develop new radiopharmaceuticals employing 223Ra has been hindered by poor availability due to the small quantities of parent actinium-227 available world-wide. The purpose of this study was to develop innovative and cost-effective methods to obtain high-purity 223Ra from 227Ac. We obtained 227Ac from two surplus actinium-beryllium neutron generators. We retrieved the actinium/beryllium buttons from the sources and dissolved them in a sulfuric-nitric acid solution. A crude actinium solid was recovered from the solution by coprecipitation with thorium fluoride, leaving beryllium in solution. The crude actinium was purified to provide about 40 milligrams of actinium nitrate using anion ex- change in methanol-water-nitric acid solution. The purified actinium was then used to generate high-purity 223Ra. We ex- tracted 223Ra using anion exchange in a methanol-water-nitric acid solution. After the radium was separated, actinium and thorium were then eluted from the column and dried for interim storage. This single-pass separation produces high purity, carrier-free 223Ra product, and does not disturb the 227Ac/227Th equilibrium. A high purity, carrier-free 227Th was also ob- tained from the actinium using a similar anion exchange in nitric acid. These methods enable efficient production of 223Ra for research and new alpha-emitter radiopharmaceutical development. Keywords: Alpha emitters, actinium-227, thorium-227, radium-223, anion exchange. INTRODUCTION cays by energetic beta (Emax = 1.15 MeV) to 223Ra. This side chain grows in quickly and gives the actinium chain a Actinium is one of the rarest, naturally occurring ele- high beta dose-rate. Because of potentially high dose and ments, and sufficient quantities of actinium radioisotopes are 227 high airborne contamination, curie quantities of Ac (milli- difficult to obtain for research. Actinium-227 is the longest- grams) must be handled and processed in a hot cell rather lived isotope of actinium (half-life = 21.8 years) and is the than in a glove box. only isotope of actinium that can be isolated in milligram or greater amounts. Actinium-227 can be obtained in trace The daughter product 223Ra has important medical appli- amounts from uranium minerals because it belongs to the cations as a therapeutic radionuclide for cancer treatment. natural 235U decay chain. Pure 227Ac metal has a specific Commercial availability of 227Ac is poor [1], and only a few activity of 2.66x103 GBq per gram. Actinium-227 can be small sources of 227Ac are known to exist in the world. Both produced synthetically by neutron irradiation of 226Ra in an 223Ra and 227Th can be generated from highly purified 227Ac. isotope production reactor via the nuclear reaction Möller et al. [2] explored the use of crystalline hybrid or- 226Ra(n,)227Ra (half-life = 42.2 minutes) 227Ac + -, and ganic/inorganic ion exchangers based on zirconium phos- by subsequent separation and purification of 227Ac. The ther- phate and phosphonate compounds for constructing a con- mal neutron cross section for the 226Ra(n,)227Ra reaction is venient 227Ac/223Ra generator system. In contrast, we inves- about 13 barns (National Nuclear Data Center, Brookhaven tigated radiochemical separations to produce 223Ra from National Laboratory; http://www.nndc.bnl.gov/). 227Ac using anion exchange chromatography in methanol- water-nitric acid solutions. Actinium-227 decays by beta-emission to 227Th (half-life = 18.7 days), which in turn decays by alpha-emission to 223Ra (half-life = 11.4 days). The remaining members of the Study Objectives decay chain have shorter half-lives and grow-in completely The purpose of this study was to develop improved ra- within a few hours. The first daughter of 223Ra is 219Rn, a diochemical separation methods for obtaining high-purity noble gas that must be carefully handled since it can cause 223Ra from 227Ac. Medical research on new applications for airborne alpha contamination in the work space. Most of the 223Ra has been hampered by poor availability of the parent members of the 227Ac decay series have gamma emissions 227Ac. To improve the availability of 223Ra, we recovered and that may cause high radiation fields. Actinium-227 also de- purified 227Ac from legacy neutron sources. The long-lived cays by alpha decay through a side chain (1.4% abundance) parent 227Ac decays through a chain of short-lived members to 223Fr (half-life = 21.8 minutes). Francium-223 de- (Fig. 1). The short-lived decay products, after 223Ra decay, contribute alpha and beta particle radiation and increase the 223 therapeutic effectiveness of Ra in medical applications. *Address correspondence to this author at the Isotope Sciences Program, Pacific Northwest National Laboratory, 902 Battelle Blvd., P7-27, Richland, Alpha-emitter Attributes for Cancer Treatment Washington 99354 USA; Tel: 509-375-5098; Fax: 509-375-5099; E-mail: [email protected]. In many instances, alpha-particle radiation excels for †Pacific Northwest National Laboratory in Richland, Washington, is oper- cancer treatment [3] compared to beta emitters and gamma- ated by Battelle for the U.S. Department of Energy. emitters, since short-range alpha particles impart straight, 1874-4729/12 $58.00+.00 © 2012 Bentham Science Publishers Production of High-purity Radium-223 from Legacy Actinium-Beryllium Current Radiopharmaceuticals, 2012, Vol. 5, No. 3 245 tional chelates and cell-targeted protein carriers [6]. A bi- functional chelate for 223Ra has been developed but has not been tested [7] in laboratory animals. Alpha emitters should have reasonably short physical half-lives, and should be compatible with targeting moiety biokinetics of the protein carriers to maximize radiation dose to cancer cells and minimize dose to the remainder of the body. Optimal physi- cal half-lives for cancer uptake and clearance biokinetics may be on the order of one to six days, and very short half- lives (such as the 46-minute bismuth-213) may be too short for many cancer-treatment applications. For commercial preparation and shipment to hospitals, physical half-lives should be longer than two or three days. Decay-chain daugh- ters should have half-lives of a few minutes or less to mini- mize daughter migration away from target sites. The alpha emitters should have imageable photon emissions to aid in Fig. (1). Actinium-227 decay chain. gamma-camera imaging and dosimetry for treatment- planning. Only a few alpha-emitters meet these criteria and short-range (40 to 70 μm) high-ionization-density (90-150 can be provided with excellent availability at reasonable keV/μm) tracks through targeted cells. In addition, one or cost. Toward these objectives, we have studied 223Ra and two direct alpha-particles traversing a cell nucleus may be 227Th as candidate radionuclides for cancer treatment. Ra- sufficient to cause cell death, and repair of sub-lethal damage dium-223 and 227Th from 227Ac may have advantages over is minimized. The practical advantages of these properties other possible alpha-emitter choices in terms of half-life, distinguish alpha-emitters from beta-particle emitters used in relative cost, availability, and chemistry (Table 1). radiopharmaceuticals for targeted radionuclide therapy [4]. Alpha emitters provide effective treatment of cancer me- Examples of Clinical Application tastases, which often lead to cancer progression. For exam- Radium-223 can be administered in the simple, un- ple, the more common beta-emitters used in radionuclide chelated chloride form (Alpharadin™, Algeta ASA; Oslo, therapy cannot as efficiently irradiate and sterilize single Norway) for treating skeletal metastases associated with ad- cells and small metastatic lesions compared to alpha- vanced prostate and breast cancer [8]. Thorium-227 can be emitters. Alpha-emitters also minimize the toxicity associ- complexed by DOTA and other ligands and linked to mono- ated with radiation therapy by focusing a more localized clonal antibodies for cell-targeted cancer therapy. Our Labo- energy distribution pattern within targeted tissues. By com- ratory is also investigating the use of new nanoparticle con- parison, radiation from beta/gamma emitters extends greater structs for 227Th and 223Ra. distances from targeted lesions, and to a greater extent, can 223 damage normal organs and tissues--thereby limiting the Acting as a calcium mimic, Ra-chloride targets new amount of activity that may be administered. Alpha emitters bone growth in and around skeletal metastases [9]. The are effective in cell-killing at low dose rates and in low tis- short-range alpha particles destroy nearby cancer cells but do sue-oxygen environments characteristic of cancerous not uniformly traverse pockets of active red marrow in trabe- growths [5]. These properties establish a scientific rationale cular bone. A treatment involves intravenous infusion of 50 for identifying and employing alpha-emitting radionuclides, KBq per kg body weight, once per month, for six months; having suitable chemical and physical properties, for appli- this protracted infusion scheme provides maximum treatment cations in cancer treatment. benefit
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