Date of Award

8-2015

Document Type

Thesis

Degree Name

Master of Science (MS)

Legacy Department

Environmental Engineering and Earth Science

Advisor

DeVol, Timothy A

Committee Member

Williams, Calvin L

Committee Member

Powell, Brian A

Abstract

An on-line radiation monitoring system that simultaneously concentrates and detects radioactivity is needed to detect an accidental leakage from a nuclear waste disposal facility or clandestine nuclear activity. Previous studies have shown that classical control chart methods can be applied to on-line radiation monitoring data to quickly detect these events as they occur; however, Bayesian control chart methods were not included in these studies. This work will evaluate the performance of a Bayesian control chart method, the Shiryaev-Roberts (SR) procedure, compared to classical control chart methods, Shewhart 3-σ and cumulative sum (CUSUM), for use in on-line radiation monitoring of 99Tc in water using extractive scintillating resin. Measurements were collected by pumping solutions containing 0.1-5 Bq/L of 99Tc, as 99TcO4-, through a flow cell packed with extractive scintillating resin coupled to a Beta-RAM Model 5 HPLC detector. While 99TcO4- accumulated on the resin, simultaneous measurements were acquired in 10-s intervals and then re-binned to 100-s intervals. The Bayesian statistical method, Shiryaev-Roberts procedure, and classical control chart methods, Shewhart 3-σ and cumulative sum (CUSUM), were applied to the data using statistical algorithms developed in MATLAB®. Two SR control charts were constructed using Poisson distributions and Gaussian distributions to estimate the likelihood ratio, and are referred to as Poisson SR and Gaussian SR to indicate the distribution used to calculate the statistic. The Poisson and Gaussian SR methods required as little as 28.9 mL less solution at 5 Bq/L and as much as 170 mL less solution at 0.5 Bq/L to exceed the control limit than the Shewhart 3-σ method. The Poisson SR method needed as little as 6.20 mL less solution at 5 Bq/L and up to 125 mL less solution at 0.5 Bq/L to exceed the control limit than the CUSUM method. The Gaussian SR and CUSUM method required comparable solution volumes for test solutions containing at least 1.5 Bq/L of 99Tc. For activity concentrations less than 1.5 Bq/L, the Gaussian SR method required as much as 40.8 mL less solution at 0.5 Bq/L to exceed the control limit than the CUSUM method. Both SR methods were able to consistently detect test solutions containing 0.1 Bq/L, unlike the Shewhart 3-σ and CUSUM methods. Although the Poisson SR method required as much as 178 mL less solution to exceed the control limit than the Gaussian SR method, the Gaussian SR false positive of 0% was much lower than the Poisson SR false positive rate of 1.14%. A lower false positive rate made it easier to differentiate between a false positive and an increase in mean count rate caused by activity accumulating on the resin. The SR procedure is thus the ideal tool for low-level on-line radiation monitoring using extractive scintillating resin, because it needed less volume in most cases to detect an upward shift in the mean count rate than the Shewhart 3-σ and CUSUM methods and consistently detected lower activity concentrations. The desired results for the monitoring scheme, however, need to be considered prior to choosing between the Poisson and Gaussian distribution to estimate the likelihood ratio, because each was advantageous under different circumstances. Once the control limit was exceeded, activity concentrations were estimated from the SR control chart using the slope of the control chart on a semi-logarithmic plot. Five of nine test solutions for the Poisson SR control chart produced concentration estimates within 30% of the actual value, but the worst case was 263.2% different than the actual value. The estimations for the Gaussian SR control chart were much more precise, with six of eight solutions producing estimates within 30%. Although the activity concentrations estimations were only mediocre for the Poisson SR control chart and satisfactory for the Gaussian SR control chart, these results demonstrate that a relationship exists between activity concentration and the SR control chart magnitude that can be exploited to determine the activity concentration from the SR control chart. More complex methods should be investigated to improve activity concentration estimations from the SR control charts.

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