The Determination of 210Pb by Accelerator Mass Spectrometry

Title: The Determination of 210Pb by Accelerator Mass Spectrometry
Authors: Sookdeo, Adam
Date: 2015
Abstract: The aim of thesis was to establish a methodology for 210Pb measurements by Accelerator Mass Spectrometry (AMS). The potential application is to measure 210Pb in people who have been exposed to radon. This will better our understanding of radon toxicity, which is not possible now with current radiometric and mass spectrometry techniques. The determination of 210Pb by AMS was done in two major studies 1) Studying Pb chemistry in a Cs+ sputter source used in AMS and 2) Evaluating 204,205 & 208Pb spikes for the quantification of 210Pb by isotope dilution. Pb chemistry was investigated using an 834 SIMS-type and a SO-110 Cs+ sputter source at the IsoTrace Laboratory and A.E Lalonde AMS facility, respectively. Different molecular anions of Pb were studied with the 834 SIMS-type Cs+ sputter source and the strongest molecular anion current of Pb and thus greatest ionization efficiency was achieved form the superhalogen PbF3-. The average 208PbF3- current was unaffected by varying the ratio of the fluorinating compounds (AgF2 and CsF) packed into a target. The average current of 208PbF3- was reproducibly increased by chemically mixing the targets of AgF2, CsF and PbF2 in concentrated HF rather than mechanically mixing them the powders with a stir rod. The count rate of 210Pb reproducibly increased by a factor of 20 when μg quantities of PbF2 were present in mg AMS targets compared to AMS targets that had pg quantities of PbF2. The average current of 208PbF3- for pure PbF2 targets in an SO-100 Cs+ sputter source was reproducibly increased when the Cs+ flux was decreased by a factor of 10. This phase of my work maximized the overall efficiency of PbF3-, to a value of 1.8x10-10 ±8x10-11s-, which was a key first step in the measurement by AMS. Then isotope dilution was tested to quantify 210Pb and the next stage of my work evaluated the use of 204,205 & 208Pb spikes. 210Pb was measured in the +3 charge state by isotope dilution assays using 204,205 & 208Pb spikes. 204Pb+3 reproducibly suffered from the molecular interference from 68Zn3+3, which could not be easily removed without negatively impacting the detection limit for 210Pb. 205Pb+3 continually suffered from 205Tl+3 interference which could be readily be removed but not without negatively affecting the II detection limit for 210Pb. 208Pb+3 suffers from no molecular interferences but if a large amount of 208Pb is needed to swamp the Pb in a sample, this could limit the detection limit for 210Pb as the abundance sensitivity is 210Pb/208Pb=1.3×10-12. A calibration curve is required when 208Pb is used as a spike due to a difference in collection efficiency of a Faraday cup, where 208Pb+3 is detected and the gas ionization chamber, where 210Pb+3 is detected. The quantification of 210Pb with 208Pb as a spike yielded a detection limit of 4.4mBq at the IsoTrace facility. A theoretical detection limit of ≤0.11mBq is expected at the A.E Lalonde AMS facility. The expected detection limit at the A.E Lalonde AMS facility is on par with α-spectroscopy but AMS samples can be counted in less than 1 hour whereas alpha spectrometry samples must be counted for about 1 day.
CollectionThèses, 2011 - // Theses, 2011 -