A solvent extraction technique has been developed for the radiochemical separation and purification of 144 Ce from Purex high-level waste (HLW). The feed solution initially was in contact with granulated ammonium molybdophosphate for the selective removal of cesium to reduce the gamma dose during the subsequent process. In the next step, uranium and plutonium were removed quantitatively by using 20% 2-ethylhexyl hydrogen 2-ethylhexyl phosphonate (KSM-17) in dodecane. The trivalent cerium present in the cesium-, uranium-, and plutonium-depleted raffinate was oxidized to its tetravalent state by using K 2 Cr 2 O 7 and was extracted into KSM-17. The loaded cerium from the organic phase was stripped with 0.5 M nitric acid. Final decontamination from 3143 trace impurities such as 106 Ru and 125 Sb could be achieved by an additional cerium-extraction step with KSM-17 at pH 2, followed by its stripping with 0.5 M HNO 3 . About 10 mCi of cerium was separated from Purex HLW by using this technique. This method is amenable for automation and scale up.
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