The Separation of 241

Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. State–of-the-art power sources generate electricity from alpha decay of 238Pu via thermoelectric conversion. However, production of 238Pu requires specialist facilities including a nuclear reactor, a source of 237Np for target irradiation and hotcells to chemically separate neptunium and plutonium within the irradiated targets. These specialist facilities are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is considered a promising alternative heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). As a daughter product of 241Pu decay, 241Am exists in 1000 kgs quantities within the UK civil plutonium stockpile. A chemical separation process is required to extract the 241Am in a pure form and this paper describes the AMPPEX process (Americium and Plutonium Purification by Extraction), successfully developed over the past five years to isolate 241Am in high yield (> 99%) and to a high purity (> 99%). The process starts by dissolving plutonium dioxide in nitric acid with the aid of a silver(II) catalyst, which is generated electrochemically. The solution is then conditioned and fed to a PUREX type solvent extraction process, where the plutonium is separated from the americium and silver. The plutonium is converted back to plutonium dioxide and the americium is fed forward to a second solvent extraction step. Here the americium is selectively extracted leaving the silver in the aqueous phase. The americium is stripped from the solvent and recovered from solution as americium oxalate, which is calcined to give americium dioxide as the final product. This paper will describe the development of the separation process over a series of six solvent extraction separation trials using centrifugal contactors. The material produced (~ 4g 241Am) was used to make ceramic pellets to establish the behaviour of americium oxide material under high temperature (1450°C) sintering conditions. The chemical separation process is now demonstrated at concentrations expected on the full scale facility taking this process to TRL 4-5

Cerium neodymium oxide solid solution synthesis as a potential analogue for substoichiometric AmO 2 for radioisotope power systems

The European Space Agency (ESA) is sponsoring a research programme on the development of americium oxides for radioisotope generators and heater units. Cubic AmO2-(x/2) with an O/Am ratio between 1.65 and 1.75 is a potentially suitable compound for pellet sintering. C-type (Ia-3) Ce1-xNdxO2-(x/2) oxides with 0.5 &lt; x &lt; 0.7 could be used as a surrogate for some Ia-3 AmO2-(x/2). A new Ce1-xNdxO2-(x/2) production process has been investigated where a nominally selected x value of 0.6 was targeted: Ce and Nd nitrates and oxalic acid were added drop-wise into a vessel, where they continuously reacted to create oxalate precipitates. The effect of temperature (25 °C, 60 °C) of the reactants (mixed at 250 revolutions per minute) on oxalate particle shape and size were investigated. Oxalates were calcined at 900 °C to produce oxide particles. Oxalate particle properties were characterised as these are expected to influence oxides particle properties and fuel pellet sintering.</p

Plutonium(VI) complexation by diglycolamide ligands coordination chemistry insight into TODGA-based actinide separations

Complexation of Pu(IV) with TMDGA, TEDGA, and TODGA diglycolamide ligands was followed by vis-NIR spectroscopy. A crystal structure determination reveals that TMDGA forms a 1 : 3 homoleptic Pu(IV) complex with the nitrate anions forced into the outer coordination sphere

The Separation of 241Am from Aged Plutonium Dioxide for use in Radioisotope Power Systems

Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. State–of-the-art power sources generate electricity from alpha decay of 238Pu via thermoelectric conversion. However, production of 238Pu requires specialist facilities including a nuclear reactor, a source of 237Np for target irradiation and hotcells to chemically separate neptunium and plutonium within the irradiated targets. These specialist facilities are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is considered a promising alternative heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). As a daughter product of 241Pu decay, 241Am exists in 1000 kgs quantities within the UK civil plutonium stockpile. A chemical separation process is required to extract the 241Am in a pure form and this paper describes the AMPPEX process (Americium and Plutonium Purification by Extraction), successfully developed over the past five years to isolate 241Am in high yield (> 99%) and to a high purity (> 99%). The process starts by dissolving plutonium dioxide in nitric acid with the aid of a silver(II) catalyst, which is generated electrochemically. The solution is then conditioned and fed to a PUREX type solvent extraction process, where the plutonium is separated from the americium and silver. The plutonium is converted back to plutonium dioxide and the americium is fed forward to a second solvent extraction step. Here the americium is selectively extracted leaving the silver in the aqueous phase. The americium is stripped from the solvent and recovered from solution as americium oxalate, which is calcined to give americium dioxide as the final product. This paper will describe the development of the separation process over a series of six solvent extraction separation trials using centrifugal contactors. The material produced (~ 4g 241Am) was used to make ceramic pellets to establish the behaviour of americium oxide material under high temperature (1450°C) sintering conditions. The chemical separation process is now demonstrated at concentrations expected on the full scale facility taking this process to TRL 4-5

The Separation of

Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. State–of-the-art power sources generate electricity from alpha decay of 238Pu via thermoelectric conversion. However, production of 238Pu requires specialist facilities including a nuclear reactor, a source of 237Np for target irradiation and hotcells to chemically separate neptunium and plutonium within the irradiated targets. These specialist facilities are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is considered a promising alternative heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). As a daughter product of 241Pu decay, 241Am exists in 1000 kgs quantities within the UK civil plutonium stockpile. A chemical separation process is required to extract the 241Am in a pure form and this paper describes the AMPPEX process (Americium and Plutonium Purification by Extraction), successfully developed over the past five years to isolate 241Am in high yield (> 99%) and to a high purity (> 99%). The process starts by dissolving plutonium dioxide in nitric acid with the aid of a silver(II) catalyst, which is generated electrochemically. The solution is then conditioned and fed to a PUREX type solvent extraction process, where the plutonium is separated from the americium and silver. The plutonium is converted back to plutonium dioxide and the americium is fed forward to a second solvent extraction step. Here the americium is selectively extracted leaving the silver in the aqueous phase. The americium is stripped from the solvent and recovered from solution as americium oxalate, which is calcined to give americium dioxide as the final product. This paper will describe the development of the separation process over a series of six solvent extraction separation trials using centrifugal contactors. The material produced (~ 4g 241Am) was used to make ceramic pellets to establish the behaviour of americium oxide material under high temperature (1450°C) sintering conditions. The chemical separation process is now demonstrated at concentrations expected on the full scale facility taking this process to TRL 4-5