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Recovery of Platinum Group Metals from High Level Radioactive Waste POSSIBILITIES of SEPARATION and USE RE-EVALUATED by R

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Recovery of Platinum Group Metals from High Level Radioactive Waste POSSIBILITIES of SEPARATION and USE RE-EVALUATED by R Recovery of Platinum Group Metals from High Level Radioactive Waste POSSIBILITIES OF SEPARATION AND USE RE-EVALUATED By R. P. Bush AEA Technology, Harwell Laboratory, Oxfordshire, England When nuclear fuel is irradiated in a power reactor a wide range of chemical elements is created by the fission of uranium and plutonium. These fission products include palladium, rhodium and ruthenium, and could in principle constitute a valuable source of these three metals. Their separation from the fuel during reprocessing operations is, however, a complex matter. Various processes have been proposed and evaluated, mainly on a laboratory scale. To date none of them has been established as applicable on a commercial scale, but investigations with this aim are continuing in several countries. Even a complete separation of the platinum group metals from other nuclides would yield a radioac- tive product, because of the presence of active isotopes of the platinum group metals. These would be expected to restrict the practical utilisation of platinum group metals created by nuclear jisswn, unless an isotope separation technique can be developed, or the metals are stored until the radioactivity has decayed. The irradiation of nuclear fuels in power reviewed in Platinum Metals Review in 1970 reactors leads to the production of atoms of a (1). The current revival of interest has resulted wide range of fission products, ranging in partly because of the increasing economic im- atomic mass from 70 to 160. These fission pro- portance of rhodium. This metal is a crucial ducts generally constitute components of the component of the three-way catalysts used for radioactive waste generated by the nuclear fuel automobile emission control, and the demand cycle. They include three of the platinum group for it is therefore strong. However, rhodium is metals, namely palladium, rhodium and mined in conjunction with platinum and its ruthenium, which are valuable because of their supply is therefore linked to that of platinum. scarcity and their strategic importance. Increases in the price of rhodium over the last It is the purpose of this paper to review the few years have led to renewed interest in possi- quantities of the platinum group elements pro- ble new sources. For this reason, the present duced (frequently termed the arisings) during paper concentrates on recent technological nuclear power generation, to describe their developments that might have a bearing on the behaviour within the fuel cycle, and to consider separation of rhodium from nuclear waste. the feasibility of separating them from suitable waste streams and utilising them industrially. Production of Platinum Metals The question of whether these metals might in Nuclear Fuel be separated from nuclear wastes was con- Palladium, rhodium and ruthenium are pro- sidered in the early days of the nuclear in- duced in irradiated fuel at fission yields of a few dustry, and interest in it has re-emerged at per cent. The quantities produced depend on intervals since then. The topic was previously the type of reactor system and on the burn-up Platinum Metals Rev., 1991, 35, (4), 202-208 202 Table I Composition of Fission Product Platinum Group Metals after Cooling for Five Years Content, Specificla' Isotope weight Half-life activity, Decay mode per cent Ci/g metal Ruthenium 99 trace stable 100 4.2 stable 101 34.1 stable 102 34.0 stable 103 trace 39 days Low PY 104 23.9 stable 106 3.8 368 days 8 Low energy P Rhodium 102 trace 2.9 years 1.3 x 10-3 y, electron capture 102m trace 207 days 3 x 10-5 by, electron capture 103 100 stable 1 061b' trace 30 seconds PY Palladium 104 16.9 stable 105 29.3 stable 106 21.3 stable 107 17.0 6.5 x lo5 years 5 x 10-6 Low energy p 108 11.7 stable 110 3.8 stable la1 1 Curie ICi) 3.7 x 1O'O Becquerel Ib) '04Rh exists in secular equilibrium with 'O'Ru. and decays rapidly to "'OPd to which the fuel is taken, that is the thermal Rhodium, currently the most valuable of the energy generated by fission by unit mass of three, is generated in the lowest yield. fuel. In a commercial light water reactor at a The isotopic composition of the fission deriv- burn-up of 33GWdhe about 4 kg of platinum ed platinum group metals is different from that group metals are produced per tonne of heavy of the natural metals; and it varies over time as metal in the fuel. In a fast breeder reactor, the fuel cools, because the radioactive isotopes because of the higher burn-up (about present are subject to decay. At the time of 100GWdlte) and the different neutron spec- discharge from the reactor a number of very trum, about 19 kg of platinum group metals per short lived isotopes are present, but these decay tonne are produced. For light water reactor rapidly. The composition after about five years fuel, the approximate composition of the is shown in Table I. With longer times the platinum group metals fraction is: palladium composition and the total masses of the 33, rhodium 11 and ruthenium 56 per cent. elements present do not vary significantly, Platinum Metals Rev., 1991, 35, (4) 203 apart from the conversion of Io6Ruto '06Pd. There is, however, an insoluble residue which Some of the isotopes shown in Table I are on- contains some of the platinum group metals. ly present at low mass concentrations, but they The acid solution is clarified and then passes to are important because they impart radioactivity a sequence of solvent extraction contactors in to the metal. This radioactivity has important which separation of uranium and plutonium implications for the potential utilisation of the from the fission products, and from each other, metals, even if they were separated. We shall is carried out. Most of the fission products in return to this point later in the paper. the dissolver solution, including the platinum In order to obtain an idea of the potential group metals, pass to the aqueous raffinate platinum group metals resource in nuclear fuel, from the first solvent extraction cycle. This raf- it is necessary to consider the size of present finate is subsequently concentrated by evapora- and future nuclear power programmes. It is tion to give high level waste liquor, which is possible to estimate the total world arisings of then stored prior to vitrification and final fission product platinum group metals from disposal. During these stages further precipita- their fission yields and the expected arisings of tion of insoluble material can occur. spent fuel based on forecasts from the Organisation for Economic Co-operation and Insoluble Residues Development (OECD) and others. Light water The insoluble material from the dissolution reactor data can be used for the calculation stage contains 70 to 90 per cent fission pro- because this type of reactor will dominate the ducts, together with miscellaneous residues and nuclear power programmes for the world as a traces of undissolved actinides. These fission whole. In Table I1 the arisings based on one set products exist as metallic alloys containing of assumptions (2) are compared with annual molybdenum and technetium as well as consumption in the World Outside Centrally- palladium, rhodium and ruthenium. About 4 to Planned Economies Area (WOCA), and with 5 kg of residues per tonne of fuel have been 1982 estimates of the world reserves. Full found in small scale tests, and fine material details of the calculations are given elsewhere (60pn) is present. The amounts and composi- (2). tions are variable, and the residues are intensely The data show that nuclear arisings of the radioactive, with heat outputs of up to lW/g. platinum group metals are potentially a signifi- The fraction of the initial inventory of cant fraction of reserves, and represent many platinum group metals which occurs in the in- years consumption at current rates. However, soluble residues depends on the burn-up to the platinum group metals content of the fission which the fuel has been taken. For high burn- product of spent fuel is not immediately up fast reactor fuel, about 98 per cent of the available to man. For the metals to become total expected ruthenium has been found in the attainable it is necessary for the fuel to be residues (3). reprocessed. It is thought likely that about half The insoluble residues are difficult to treat the nuclear fuel from power reactors world- chemically because of their inertness, and their wide will be reprocessed (2). high radioactivity adds to the difficulty and ex- pense of processing them. Direct high Behaviour of Platinum Group temperature chlorination, or alloying with tin, Metals during Fuel Processing has been used to bring the residues into solu- When spent nuclear fuel is reprocessed, the tion for analytical purposes (4). It is unlikely, fuel pins are sheared into short lengths, and the however, that such methods could be scaled up fuel is dissolved away from the cladding into economically. 7M nitric acid. During this operation, the High temperature processes that are based on uranium and plutonium oxides that are present extraction with liquid metals have been propos- dissolve, as do most of the fission products. ed. For example, molten uraniudchromium or Platinum Metals Rev., 1991, 35, (4) 204 uraniumhron eutectics extract ruthenium selec- Table I, it is clear that ruthenium-106 and its tively from a solution of the residues in molten daughter rhodium-I06 are the main con- magnesium (5). More recently, Japanese in- tributors to the radioactivity of the platinum vestigations have shown that treatment of the group metals fraction. The separation of residues with lead and a glass-forming material ruthenium from rhodium and palladium might causes extraction of the platinum group metals therefore be a worthwhile objective, perhaps as together with technetium and molybdenum, in- a preliminary step to the purification of the to the lead phase, leaving other impurities in rhodium and palladium.
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