Abstract
A sequential extraction method consisting of six operationally-defined fractions has been developed for determining the geochemical partitioning of natural (U, Th, 40K) and antropogenic (Pu, Am, 137Cs) radionuclides in a 40–50 cm deep sediment sample collected in a Venice canal. Extraction chromatography with Microthene-TOPO (U, Th), Microthene-TNOA (Pu) and Microthene-HDEHP (Am) column was used for the chemical separation of a single radionuclide; the final recoveries were calculated by adding 236U, 229Th, 242Pu and 243Am as the yield tracers. After electrodeposition the alpha spectrometry was carried out. 137Cs and 40K were measured by gamma spectrometry. The total concentrations in the wet sample (Bq/kgd), obtained by a complete disgregation of the matrix by wet and dry treatment, were the following: 239+240Pu=1.03±0.07, 238Pu=0.022±0.005, 241Am=0.337±0.027, 137Cs=9.78±0.78, 238U=28.84±1.62, 232Th=21.42±1.93, 40K=376.05±12.78. The mean ratio 238Pu/239+240Pu (0.02) shows a contamination due essentially to fall-out and U and Th alpha spectra indicate the natural origin of two elements. The absence of 134Cs in the sample proves that at 40–50 cm depth the sediment was not affected by the Chernobyl fall-out. As far as the speciation is concerned the following fractions were considered: water soluble, carbonates, Fe−Mn oxides, organic matter, acid soluble, residue. Pu (∼67%) an Am (∼95%) were present principally in the carbonate fraction; U was more distributed and about 30% and 45% appeared in the carbonate fraction and in the residue respectively; the majority of Th was present in the residue (∼60%); 40K was totally present in the residue; finally 137Cs was found mostly in the acid soluble fraction (∼53%) and in the residue (∼47%). Some stable elements (Fe, Mn, Al, Ti, Ca, Pb, Ba) were also determined in the different fractions to get more information about the chemical association of the single radionuclides.
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