Separation of U and Pu in spent nuclear fuel sample using anion-exchange-group-introduced porous polymer sheet for ICP-MS determination

Abstract

Anion-exchange porous sheets were prepared by radiation-induced graft polymerization and subsequent chemical modifications. A diethylamino (DEA) group as an anion-exchange group was introduced into the polymer chain grafted onto a porous sheet. The DEA group-introduced porous sheet was cut into disks 13 mm in diameter and 3 mm in thickness to fit an empty cylindrical cartridge (DEA cartridge). The DEA sheet had a DEA group of 3.4 mol/kg of the DEA-group-containing porous sheet and a linear velocity of 46 m/h at a permeation pressure of 0.1 MPa at 298 K. The adsorption capacity of the DEA cartridge for FeCl 4 − as a model ion in equilibrium with 1 g-Fe(III)/L in 10 M HCl was 0.17 mmol-Fe(III)/DEA cartridge. No Pu leakage during the permeation of 5 mL of 10 M HCl–0.1 M HNO 3 containing Pu ionic species through the DEA cartridge was observed irrespective of the permeation rate ranging from 0.3 to 80 mL/min. A solution containing known amounts of 233U, 240Pu, and 241Am in 10 M HCl–0.1 M HNO 3 was loaded onto the DEA cartridge. U and Pu were retained on the DEA cartridge, while Am was allowed to pass through the DEA cartridge. Subsequently, 7 M HNO 3 and 1 M HCl as eluents were permeated to elute U and Pu from the DEA cartridge, respectively. The decontamination factor of U in a Pu fraction, defined by dividing the activity of U in the feed solution by that of U in the Pu fraction, was 2.7 × 10 5, which is desirable for the highly accurate ICP-MS determination of Pu for samples containing both U and Pu. The method using the DEA cartridge was validated by measuring isotopic compositions and quantities of U and Pu in a spent nuclear fuel sample by double-focusing magnetic sector ICP-MS.