Ceramic conversion and densification of zirconium phosphonate sorbent materials

2019 
Abstract The simple conversion of zirconium phosphonate sorbent materials, with known affinity for lanthanide elements, to durable ceramic waste forms via thermal treatment has been demonstrated. The use of zirconium phosphonate enables both removal of targeted elements from spent nuclear fuel and immobilisation into leach resistant solid products to be achieved using a single material. Thermal conversion was performed on the zirconium phosphonate both before and after loading with europium, which acted as a surrogate for the chemically similar minor actinides. Without europium loaded, the zirconium phosphonate sorbent formed predominantly KZr 2 (PO 4 ) 3 upon heating, independent of the processing conditions used. A maximum relative density of 87% was achieved with cold isostatic pressing (200 MPa) and sintering at 1200 °C for 12 h. When the zirconium phosphonate sorbent was loaded with europium, the phase composition formed upon thermal treatment was more complex. Specifically, mixtures of ZrP 2 O 7 , Eu 0.33 Zr 2 (PO 4 ) 3 , EuPO 4 and Zr 2 O(PO 4 ) 2 were formed, with phase compositions depending on the temperatures and pressures used. The simplest phase composition for the europium loaded material was achieved via uniaxial pressing (120 MPa) and sintering at 1300 °C for 1 h, although the ceramic pellet produced under these conditions had a relative density of only 53%. The loaded europium deported primarily to a EuPO 4 phase, which is known to be highly stable and leach resistant. As such, these zirconium phosphonate materials have potential utility for treatment of nuclear wastes.
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