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Radiochemistry of Germanium

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Radiochemistry of Germanium Jointly published by Journal of Radioanalytical and Nuclear Chemistry, Articles, Elsevier Science S. A., Lausanne and Vol. 202, Nos 1-2 (1996) 7-102 Akaddmiai Kiad6, Budapest Renew RADIOCHEMISTRY OF GERMANIUM S. MIRZADEH,* R. M. LAMBRECHT** *Nuclear Medicine Group, Oak Ridge National Laboratory, Oak Ridge, TN, 37830 (USA) **Biomedicine and Health, Australian Nuclear Science and Technology Organisation, Menai,NSW (Australia) (Received March 13, 1995) Contents 1. Some general information 9 1.1 Natural occurrence 9 1.2 Environmental concentrations 13 1.3 Toxicity 14 1.4 Applications 15 2, General review of the inorganic and analytical chemistry of germanium 16 2".1 Germanium metal 16 2.2 Germanium compounds 19 a. Hydrides 21 b. Halides 22 c. Oxides 23 d. Sulfides 23 e. Organometallic compounds 24 2.3 Electrochemistry 25 2.4 Detection of germanium 25 a. Activation analysis 26 3. Production of germanium radioisotopes 27 4= A summary of the chemical behavior of carrier-free germanium-68 32 5, Hot-atom chemistry of germanium 34 6. Separation methods 38 6.1 Volatilization and gas chromatography 39 6.2 Precipitation and coprecipitation 41 a. Reaction with hydrogen sulfide 41 b. Coprecipitation with acid-insoluble sulfides 42 c. Coprecipitation with hydroxides of group III elements 43 0236-5731196/US $ 32.0 Copyright 1996 Akad#miai Kiad6, Budapest All rights reserved S. M1RZADEH, R. M. LAMBRECHT: RADIOCHEMISTRY OF GERMANIUM 6.3 Extraction 44 a. Extraction with organic solvents 44 b. Extraction of germanium complexes 48 c. Extraction with hydroxyl-containing organic ligands 51 6.4 Ion-exchange chromatography 52 a. Cation exchange 53 b. Anion exchange 56 c. Adsorption on inorganic exchangers 59 d. Thin-layer and paper chromatography 62 6.5 Electrodeposition 66 7. Applied radiochemistry o! germanium 67 7.1 68Ge--~6eGagenerator in biomedical research 67 7.2 71Ga[v,fl]71Ge: A radiochemical detector for the solar neutrino 72 8. Selected radiochemical procedures 75 8.1 Separation of germanium radioisotopes from various media 76 a. Fission products 76 b. Proton-irradiated RbBr target 76 c. Proton-irradiated Ga metal target 78 d. Proton-irradiated Ga4Ni target 79 8,2 Rapid separation of germanium isotopes from fission products 80 83 Determination of germanium by neutron activation 81 8.4 Thin-layer chromatographic separation of carrier-free 77As from 77Ge 82 References 85 Since the publication of Radiochemistry of Germanium_ (NAS-NS-3043) in 1961, there have been significant developments on the subject. During the period from 1970 to 1980, the diagnostic utilization of the 68Ge--.6SGagenerator system in nuclear medicine stimulated research in the field. In addition, over the past 30 years there have been many advances in the analytical chemistry of germanium (Go), owing to the rapid increase in application of Ge in the electronics industry and, most recently, as an important component in infrared spectrometers. This latest review has been completely rewritten. A literature search has been completed through December of 1990. Literature for selected topics has been surveyed through September 1993. The first section contains general information about germanium and its radioisotopes, and relevant nuclear data in tabulated form. in the second section, a general review of the inorganic and analytical chemistry of Ge is presented. Following these two introductory sections, subsequent sections deal with the production and preparation of germanium radioisotopes, separation and determination of Ge, of particular interest to the radiochemist, and selected procedures for its determination in or separation from various media. The section on separation chemistry has been greatly expanded. The review includes sections on hot-atom chemistry and the chemical behavior of carrier-free 68Ge. A section entitled "Applied Radiochemistry of Germanium" deals specifically with 68Ge .._.68 Ga generator systems, the role of 71Ge in the detection of solar neutrinos, and the preparation of 68Ge positron sources for studying dislocations in metallic lattices and calibration of Positron Emission Tomography (PET) cameras. Two other noteworthy points follow. Throughout the text, the oxidation state of a metal ion having only one stable state, such as germanium, is not explicitly indicated. Therefore, "Go" typically represents Ge4+, Other ions such as arsenic and tin, however, are indicated with their appropriate oxidation states. The term "carrier-free" applies to radioactive preparations to which no isotopic carrier (stable isotopes) is intentionally added. S. MIRZADEH, R. M. LAMBRECHT: RADIOCHEMISTRYOF GERMANIUM 1. Some General Information 1~.1. Natural Occurrence 1.2. Environmental Concentrations 1.3. Toxicity 1.4. Applications 1.1 Natural Occurrence Germanium (Ge) is a semiconducting metalloid of the Group IVA elements. It was predicted and called eka-silicon by Mendeleef, and was discovered in 1886 by Clemens Winkler. It is grayish-white, lustrous and brittle like glass. It is diamond-cubic in structure when crystalline. Germanium and many of its alloys expand on solidification. There are five stable isotopes of germanium: 7~ (20.55%), 72Ge (27.37%), 73Ge (7.67%), 74Ge (36.74%) and 76Ge (7.67%). A recent measurement of the isotopic abundance of Ge in a range of terrestrial materials using solid-source mass spectrometry revealed no variations in isotopic abundances in any of the reagents or minerals analyzed. 1 Among the nineteen known radioisotopes of germanium, seven are proton-rich and decay with I~+ and/or electron capture (64Ge - 71Ge with 7~ being stable), and nine radioisotopes are neutron-rich and decay by iT (75Ge - 84Ge with 76Ge being stable). There are only four very short-lived metastable isotopes of germanium: 71rnGe, 75raGe, 77mGe and 79mGe. Of the four, the last three are neutron-rich. Germanium-68, with a half-life of 270.8:t:0.3 days, is the longest-lived radioisotope of germanium. A summary of the nuclear and decay data pertaining to germanium isotopes and their production is given in Tables 1.1 and 1.2. The neutron capture cross sections for germanium isotopes and a summary of the fission neutron-averaged cross sections for [n,p], [n,a] and [n,2n] reactions are given in Tables 1.3 and 1.4, respectively. The data have been taken from references 2-59. On a cosmic scale, germanium occurs as a trace element in iron meteorites, in stony meteorites, in the sun, and in the stars. The cosmic abundance of Ge is ~50 atoms per lx106 atoms of silicon. The crust of the earth is estimated to contain 1-2 g Ge per ton, or 1-2 ppm, so it is somewhat more abundant than gallium and lead, but less abundant than arsenic, beryllium, boron and bromine. Ge is not found in the free state on e~lrth, but always in combination with other elements. It may be found as argyrodite, a sulfide of germanium and silver, germanite, which contains 8% of the element, in zinc ores, and in other minerals. It also occurs in significant concentrations (up to 2-8 ppm) S. MIRZADEH, R. M. LAMBRECHT: RADIOCHEM]STRY OF GERMANIUM 09 (D 46 r~ O. ~ ~ E LLI~, > LLI~, ~) I',- 04 , , ~ , ~ ~ ~ ~, "0 0 E O v o4 (.(9 (.O O .-'2 O ~0 E 04 00 co r '-,O .=_ I.O (O O~ fo O~ 0,4 O') o eO 09 09 c~l 04 C~l 04 o e- "- E -o -':: ~ ~'~ "O e, (o cO QO tO t.O I'..- O') ~ I'-. (D 05 O tO ,,r- t",,I z T- t.O tO I'-.- OO CO CD I-- C (D tD ",.O tO .r r 1"-- 10 S. MIRZADEH, R. M, LAMBRECHT: RADIOCHEMISTRY OF GERMANIUM O~ O. 0 c~ tU~ > ~0~ ~ g~, O'~ t.O o>~ ~ ~ o~ r-- r e,i O'~ , + O') 0 O O v ,0J O I-- .m I--- o0 t,D "r "r to r r..,- o o,,I ~ r o") t'N c~l CN L= t- Z I ~-= E E mB ~ t.O r I'--- I'..- 1I S. MIRZADEH, R. M. LAMBRECHT: RAD1OCHEMISTRY OF GERMANIUM s s (N A > && c~o W~ o') 0 og 0 0 oo I- ,+ -I- + 0 CO 0 0 o , +o +o 0 v > 19 Q, u~ 0,) (0 o 0 , co ~ ,..o co a,. IM E < ~o I,N 0 0 > , O) 0') O) ~E i I i II O0 =O E o~ gl o. t~ tg~ (D t'~ t'~ O') 05 O z x (9 0~ e~ CO c'q t"o r~m s Fo t~ .el o 12 S. MIRZADEH, R. M. LAMBRECHT: RADIOCHEMISTRY OF GERMANIUM Table 1.2 Production reactions Atomic Production Atomic Production number reactions Ref. number reactions Ref. 64 64Zn[3He,3n] [28] 73m 73As (1~---.) [50] 54Fe[12C,2n] [29] 75 74Ge[n,y] [47] 65 64Zn(3He,2n) [30] 75As(n, p) [48] 4~ [31] 75m 74Ge[n,7] [47] 66 64Zn[a,2n] [32-34] 75As[n,p] [51] 64Zn(3He,n) [35] 76Ge(n,2n) [2] 56Fe(t2C,2n) [2] 77 76Ge[n,y] [47] 67 64Zn[a,n] [36] [37] 77m 7SGe[n,y] [47] 68 66Zn[a,2n] [38] 78 82Se[n,en] [2] Zn[a, xn] [39] fission [52] 69Ga[p,2n] [40] Ga[p ,xn] [41 ] 79a fission [53,54] Ge[p,pxn] [42] Y,Rb,Br,As[p,spall] [43,44] 79b [n,a], [55] fission [53-58] 69 69Ge[d,2n] [45] Co[ C,pn] [2] 81 fission [53-58] Ga[p,xn] [2] 7~ [2] 82 fission [53-58] 71 7~ [47] 83 fission [53-58] 71Ga[d,2n] [48] 72Ge[n,2n] [46,49] 84 fission [53-58] in many coals of the world, Germanium is recovered worldwide as a byproduct of production of other metals, primarily zinc, copper and lead. Production of germanium in the U.S.
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