Publications
Potential application of microsensor technology in radioactive waste management with emphasis on headspace gas detection
Waste characterization is probably the most costly part of radioactive waste management. An important part of this characterization is the measurements of headspace gas in waste containers in order to demonstrate the compliance with Resource Conservation and Recovery Act (RCRA) or transportation requirements. The traditional chemical analysis methods, which include all steps of gas sampling, sample shipment and laboratory analysis, are expensive and time-consuming as well as increasing worker's exposure to hazardous environments. Therefore, an alternative technique that can provide quick, in-situ, and real-time detections of headspace gas compositions is highly desirable. This report summarizes the results obtained from a Laboratory Directed Research & Development (LDRD) project entitled 'Potential Application of Microsensor Technology in Radioactive Waste Management with Emphasis on Headspace Gas Detection'. The objective of this project is to bridge the technical gap between the current status of microsensor development and the intended applications of these sensors in nuclear waste management. The major results are summarized below: {sm_bullet} A literature review was conducted on the regulatory requirements for headspace gas sampling/analysis in waste characterization and monitoring. The most relevant gaseous species and the related physiochemical environments were identified. It was found that preconcentrators might be needed in order for chemiresistor sensors to meet desired detection {sm_bullet} A long-term stability test was conducted for a polymer-based chemresistor sensor array. Significant drifts were observed over the time duration of one month. Such drifts should be taken into account for long-term in-situ monitoring. {sm_bullet} Several techniques were explored to improve the performance of sensor polymers. It has been demonstrated that freeze deposition of black carbon (CB)-polymer composite can effectively eliminate the so-called 'coffee ring' effect and lead to a desirable uniform distribution of CB particles in sensing polymer films. The optimal ratio of CB/polymer has been determined. UV irradiation has been shown to improve sensor sensitivity. {sm_bullet} From a large set of commercially available polymers, five polymers were selected to form a sensor array that was able to provide optimal responses to six target-volatile organic compounds (VOCs). A series of tests on the response of sensor array to various VOC concentrations have been performed. Linear sensor responses have been observed over the tested concentration ranges, although the responses over a whole concentration range are generally nonlinear. {sm_bullet} Inverse models have been developed for identifying individual VOCs based on sensor array responses. A linear solvation energy model is particularly promising for identifying an unknown VOC in a single-component system. It has been demonstrated that a sensor array as such we developed is able to discriminate waste containers for their total VOC concentrations and therefore can be used as screening tool for reducing the existing headspace gas sampling rate. {sm_bullet} Various VOC preconcentrators have been fabricated using Carboxen 1000 as an absorbent. Extensive tests have been conducted in order to obtain optimal configurations and parameter ranges for preconcentrator performance. It has been shown that use of preconcentrators can reduce the detection limits of chemiresistors by two orders of magnitude. The life span of preconcentrators under various physiochemical conditions has also been evaluated. {sm_bullet} The performance of Pd film-based H2 sensors in the presence of VOCs has been evaluated. The interference of sensor readings by VOC has been observed, which can be attributed to the interference of VOC with the H2-O2 reaction on the Pd alloy surface. This interference can be eliminated by coating a layer of silicon dioxide on sensing film surface. Our work has demonstrated a wide range of applications of gas microsensors in radioactive waste management. Such applications can potentially lead to a significant cost saving and risk reduction for waste characterization.