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Chemical Properties of Actinium

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Chemical Properties of Actinium ••1 1 PRODUCTION AND APPLICATIONS OF *^Ac T U L.H. BAETSLE, A. DROISSART L' U C L • June 1973 I BLG 483 144, avenu* E. FUsky, BRUXELLES 4 E. PlMkylufl 144, ÏÏKV3$tL 4 (BELGIQUE) CWLOU) ..H. '-ET5LE., *. Df*OiwjAST 'il G 40 ;, jun» J.^1 '', • Df»ODUCTiC;' i»1;. -BPL'C-TIJN5 Or '"-'*': jummir^. - i'>»r i sho't survey o* ">e TI a i n c n ew i c * I ana nuclear properties "* -c 'he earlier develoDed o rodu'. t i on tec^niiu'5 are reviewed. The 'jraime- ^cjle nroluc*!on o* ii'-'^c is tised on *he irraaia'ion of la'ge amounts o' o, ; r, «he 8^ reactor. r In tkt n0» call facilities '"e irradiât ei targets -tre reo'0cesses us ng o rec i o • t-s t i on and ion e»cKançe •echnriues. The 'unction o* the radon ad- s o r o • i o " in< ventilation facility is described schematically as it takes oart in 'h» hot ce' ' operations. *ctinium-227 can be used as heat source cr in conjunction with Be as neutrcn source. The isotooic heat source oro- Traiime ai^s at the development of ! t^er-noionic jon*er*er. The neutron sources orogrjinfne coiDrises the production o* 10 to 10 ns" sources and an evaluation c* their use in oil well logging, on-line activation analysis, and neutron radiography. L.M. 3AETSLE, A. QROISSART 3LG 483 «June 1973) PRODUCTION AND APPLICATIONS OF 227Ac Î11Î.1 v.2ilin2' ~ ** een '•orte opsomming van de voornaamste chemische en nukleai-e eigenschaocer van Ac, wordt een overzicht gegeven van de reeds eerier ontwikkelde produktietechnieken. Ce gram-schaal produktie vin 22?Ac 22 is gebazeert op de bestraling van grote hoeveelheden 6fta ;n reaktor BR2. in de hete cel installaties worden de bestraalde kapsules opgewerkt door •uiddel van o ree i p i t a ti e- en ionenmisselingstechnieken. Oe funktie van de radonadsorotie- en ventiIatie-eenheid wordt schematisch beschreven zoals ze ootreedt in de hete-cel ooera+ies. Actinium-227 kan gebruikt worden als A-i TT, têS ror, of, samen ret 3e, .-* i s n eu t ronen b ron. Het ï sot*pei»-wa rmtet ron pro­ gramma beoogt de ontwikkel ing van een termoionische omzetter. Het neutronen- o o _ i cronnen orogramma omvat de oroduktie van 10 tot 10 ns bronnen en een evaluatie van hun gebruik in o Iiebron-"logging", on-line aktiveringsanal y se en neutronerradiogra'ie. L.H. BAET5LE, A. DR0ISSART BLG 483 (June 1973) PRODUCTION AND APPLICATIONS OF 227Ac R£sum4. - Après un bref aoerçu des principales propriétés chimioues et nuclé­ aires de l'Ac, les techniaues de production développées antérieurement sont résumées. La production de 'AC à l'écheMe du gramme es» basée sur l'ir­ radiation de grandes Quantités de 2°Ra dans le réacteur 6R2. Les 'bibles irradiées sont retraitées dans les installations de la cellule :h aude en utiIi sant I es t PRODUCTION AND APPLICATIONS OF 227Ac L.H. BAETSLE, A. DROISSART* June 1973 BLG 483 Work performed in association with UNION MINIERE, 1 rue de Is Chancellerie, 1000 Brussels ACTINIUM Introducti on The element actinium received its ^ame from André Louis Deb ier^e '1: in 1633 bur was really identified as a rare earth like element cy criedrich Qskcir Giesel •'2 ) in 1902. It was found in the residues T1 * the 'J ores I pitch bien a e] associated with thorium and rare earths . The honour of having separated actinium devolves upon Gtto Hahn (3j in 190S who discovered that almost all the radiation asso­ ciated with actinium comes from its decay products. The controversy about this discovery has recently been related by H.W. Kirby (4) who showed how both scientific logic and intuition were necessary to cer­ tify the existence of this "ray less" element. Extensive reviews of the earlier literature were published Dy Hagemann ,' 7) and more recently Kirby (6) reviewed the analytical chemistry of actinium and included unpublished work from the lound Laboratories. Boussieres (5) reviewed the general chemistry of actinium. Chemical properties of actinium Actinium is the first element of the actinide series and has a chemical behaviour which is almost identical to that of lan- tnanum tse lightest member of the lanthanide series. The physico-chemical data of actinium and lanthanum are summarized in Table I V?)(8 ) . It is clear from this comparison that it is extremely difficult to separate actinium from lanthanum but explains on the other nand why actinium was always found in the rare earth fraction o* the pitchblende residues. Nuclear properties of the actinium isotopes All the isotopes of actinium are racioactivo with half-lives ranging from 1 s to 2 1.77 y as summarized in Table II. It is of : 2 course oriy <- 7 /\ c w-;t,n the 21.77 y half-life which if?, of technological interest. ^'Ac constitutes a radionuclide of the 4 n • 3 series (see Fig.';. Actinium-227 itself is a we?k 0 emitter with only 1.4 % 27 a emission Dut its daughter products ^ 7r (13.73 d; and 223R3 ^11.43 d) anc other short-lived Daughters are at tne origin of a substantial amount 0*" ot, _ Ö and y radiation. The radioactive families of 2 2 6R3 p ;4n+2 rjn,± 228)-p (4n) are shewn in i£. 2 and 3. 3. PRODUCTION OF ACTINIUM Historical developments It is striking that apart from the preparations of trace quantities of actinium by Marie Curie (9) using precipitation and fractional crystallization processes no substantial progress was made until Peterson (10) produced Ac artificially in 1945 b^ irrad­ iation of 1 mg radium. When Hagemann (11) irradiated 1 g of Ra in 1949 he obtained for the first time 1.8 mg Ac free of rare earth. By using TTA extraction a 95 % pure Ac fraction was obtained. When irradiating larger quantities of Ra in reactors with higher neutron fluxes cation exchange techniques were used more and more frequently (12) (13)» From 1963 on, a research programme was started at Union Minière in conjunction with the BR2 reactor staff of S.C.K./C.E.N. in order to evaluate the possibilities of the BR2 reactor for Ac production from irradiated radium. In September 1965 Union Minière has undertaken the irradiation of 5 g 226Ra followed by separation and purification experiments ; the purification of Ac being committed to the S.C.K./C.E.N. (18). When it was decided in 1967 to start in Belgium a gram bcale Ac production programme the need for new separation techniques working in highly irradiating medium was urgently f^lt. Belgian production programme Union Minière, Brussels, and the Belgian Nuclear Research Centre S. C. K./C. E . IM. , have undertaken together the gramme-scale production of actinium at the Mol laboratories. The following important facilities are available ; 1. the high flux BR2 reactor with a neutron flux of 3 to 14 _ 4.10 n cm-2 s 1* 2. the LMA processing laboratories with hot cells equipped for work with radon; 3. the radiochemical analysis laboratories for production control. With these facilities it is possible to produce about 10 g of 227Ac per year. y croducti -, i- i-i • of radi ce e., s a:: :hs T o owi n, reactions C' v -^ 2? k ?r> 1 / ? : {Yi y; / O o o 97 8 30 c o ö >u? 4 c? 6.13 /- VT V ) 2 2.1 fc 22i? 2 25 Th r* Y; Detailed studies about the nu-clear transformation- were made at different institutes all over the world '14) Hi)(16) out the most pragmatic and practical results were obtained at S.C.K./ ci tne first, production campaign o* I9 60-197G Cl/). It may be stated that a yield of about ".C t * -> s- U i. I ~>u and G. 3 to C.4 % 2 2 8 7 (-, may he retained at an integrated flux o* 2 te 3.*û':'1 nvt. In a few cases we have observed a slightly higher transformation yield which would point at a contribution of the epitHerrr,a 1 neutrons. However, loading of the fi R 2 reactor being modified at each cycle.unexpected variations occur in the production y i e 10 measured en each individual capsule?. But the oraer of magni­ tude o^ the nuclear reaction products 2 2 / /\ c ancj 2,d8jn ^ c not change. he capsules contain between 30 and 5C g of Ra (as RaCO ) each and contain after two irradiation cyclec s the following approxi- 227 mate a• vities : 30 0 ttoo 5500 CCii 226^QRaRa,, 26 to 4 3 Ci Pc and 7 0 to 10 Ci • 228Tn. £ny chemical processing of irradiated targets must take into account these basic data and must be flexible enough to be adaptée to the activity level. CHEMICAL R 0 C E S S I G 0 F IRRADIATED RADIUM The chemical treatment of irradiât 3d racium targets has been gradually adapted "c the amount of radioactivity involved. TA extraction 1 1 J gaje satisfactory results when irradiât i n g 1 g c f R a a n c p u i' layin:vineg 11 iïiE of Ac but ne success f u a n d quanti ta tive separations wart reported afterwards (6) (18, By chemical precipitation techniques it is possible to separate Ra from Ac and Th. Several separation techniques have beer. eraposed : Ra as Ra C N0 80 HNO. (18) 3'2 in Th (10 ) in 2 M HNO (19) h as { Th (0XJ„ in 2 M HNO^ as Ac9 ( 0 X ] _ in dilute acid (20) We have found that the Ra(NC3) precipitation is an excellent and selective method to separate Ra from almost all other elements except Ba.
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