ABSTRACT
N values are routinely introduced in photon activation analysis (PAA) as the ratio of special activities of product nuclides to compare the relative intensities of different reaction channels. They determine the individual activities of each radioisotope and the total activity of the sample, which are the primary concerns of radiation safety. Traditionally, N values are calculated from the gamma spectroscopy in real measurements by normalizing the activities of individual nuclides to the reference reaction [58Ni(γ, n)57Ni] of the nickel monitor simultaneously irradiated in photon activation. Is it possible to use photon flux simulated by Monte Carlo software to calculate N values even before the actual irradiation starts? This study has applied Geant4 toolkit, a popular platform of simulating the passage of particles through matter, to generate photon flux in the samples. Assisted with photonuclear cross section from IAEA database, it is feasible to predict N values in different experimental setups for simulated target material. We have validated of this method and its consistency with Geant4. Results also show that N values are highly correlated with the beam parameters of incoming electrons and the setup of the electron-photon converter.
ABSTRACT
Batch sorption experiments were conducted with 0.5-50 ppb 99Tc, 133Cs, 237Np and U in the presence and absence of citrate and/or oxalate in a 25 g/L Savannah River Site (SRS) soil suspension. Citrate and oxalate were the ligands of choice due to their relevancy to plant exudates, the nuclides were selected for their wide range of biogeochemical behavior, and the soil from SRS was selected as a model Department of Energy (DOE) site soil. Batch samples were continually mixed on a rotary shaker and maintained at a pH of approximately 5. Analysis via ICP-MS indicated that sorption of 237Np increased with ligand concentration compared to baseline studies, as did sorption of 99Tc although to a lesser extent. The increased sorption of 237Np is proposed to be due to a combination of factors that are dependent on the ligand(s) present in the specific system including, ligand dissolution of the soil by citrate and formation of tertiary soil-oxalate-Np complexes. The increased 99Tc sorption is attributed to the dissolution of the soil by the ligands, leading to an increase in the number of available sorption sites for 99Tc. Uranium sorption decreased and dissolution of native uranium was also observed with increasing ligand concentration, thought to be a result of the formation of strong U-ligand complexes remaining in the aqueous phase. The majority of these effects were observed at the highest ligand concentrations of 50 mgC/L. No notable changes were observed for the 133Cs system which is ascribed to the minimal interaction of Cs+ with these organic ligands.
