Determination of uranium, plutonium and americium in soil and sediment by a sequential separation procedure using a sing

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Determination of uranium, plutonium and americium in soil and sediment by a sequential separation procedure using a single DGA column Nóra Vajda1   · Márton Zagyvai2 · Judit Groska1 · Edit Bokori1 · Zsuzsa Molnár1 · Mihály Braun3 Received: 2 June 2020 © Akadémiai Kiadó, Budapest, Hungary 2020

Abstract A novel method has been developed for the simultaneous determination of uranium, plutonium and americium nuclides in soil and sediment samples up to 5 g. Samples are destroyed by fusion with sodium hydroxide. Pre-concentration procedure tailored to the extraction chromatography is based on co-precipitation of actinides and removal of silica, iron and calcium. For the sequential separation of actinides a single DGA r­ esin® (containing N,N,N′,N′-tetra-n-octyldiglycol-amide) column is used. Separation of americium from lanthanides is inherently involved in the EC procedure. Alpha sources are prepared from the individual actinides strip solutions. High recoveries (above 75%) and sensitivities (about 0.1 Bq/kg) have been obtained to allow the determination of actinides of environmental levels. The whole procedure can be performed in 2 days. Keywords  Uranium · Plutonium · Americium · Soil · Sediment · DGA resin · Lanthanides

Introduction A great variety of procedures for the selective separation of major and minor actinides (Pu, U, Th, Np, Am and Cm) and their determination by α spectrometry (AS) or mass spectrometry (MS) have been described and compiled in the excellent book of Lehto and Hou [1]. Ion exchange chromatography, liquid–liquid extraction and extraction chromatography (EC) have been successfully applied for the separation of single actinides or groups of them, but there are a few methods for the combined determination of all actinides. Since a great variety of specific resins became commercially available, e.g., by EiChrom Technologies [2] and TRISKEM International [3], coupling of chromatographic columns became a standard tool for developing combined procedures. A more economic and simpler solution is offered by the use of a single resin of sufficiently high selectivity * Nóra Vajda [email protected] 1



RADANAL Ltd., Konkoly‑Thege M. út 29‑33, 1121 Budapest, Hungary

2



Centre for Energy Research, Konkoly‑Thege M. út 29‑33, 1121 Budapest, Hungary

3

ISOTOPTECH Rt., Piac u. 53, 4025 Debrecen, Hungary



where all actinides are retained on the resin followed by their sequential elution. Tetravalent actinides (Th, Pu, Np and U after oxidation state adjustment) are specifically retained by anion exchangers, TEVA (aliphatic quaternary amine), TK200 (trioctylamine), UTEVA (dipentylpentyl phosphonate), TRU (carbamoylmethyl phosphine oxide derivative) or DGA (N,N,N′,N′-tetraoctyldiglycolamide) resins. Tetraand hexavalent actinides (Th, Pu, Np and U) are specifically retained by UTEVA, TRU and DGA resins. For the selective retention of trivalent actinides (Am, Cm, Pu after reduction) two resins are potentially applicable, TRU and DGA, but DGA is superior to TRU regarding the significantly higher capacity fa