Materials Degradation and Detection (MD2): Deep Dive Final Report

An effort is underway at Pacific Northwest National Laboratory (PNNL) to develop a fundamental and general framework to foster the science and technology needed to support real-time monitoring of early degradation in materials used in the production of nuclear power. The development of such a capability would represent a timely solution to the mounting issues operators face with materials degradation in nuclear power plants. The envisioned framework consists of three primary and interconnected “thrust” areas including 1) microstructural science, 2) behavior assessment, and 3) monitoring and predictive capabilities. A brief state-of-the-art assessment for each of these core technology areas is discussed in the paper

FY06 Annual Report: Amorphous Semiconductors for Gamma Radiation Detection (ASGRAD)

We describe progress in the development of new materials for portable, room-temperature, gamma-radiation detection at Pacific Northwest National Laboratory at the Hanford Site in Washington State. High Z, high resistivity, amorphous semiconductors are being designed for use as solid-state detectors at near ambient temperatures; principles of operation are analogous to single-crystal semiconducting detectors. Amorphous semiconductors have both advantages and disadvantages compared to single crystals, and this project is developing methods to mitigate technical problems and design optimized material for gamma detection. Several issues involved in the fabrication of amorphous semiconductors are described, including reaction thermodynamics and kinetics, the development of pyrolytic coating, and the synthesis of ingots. The characterization of amorphous semiconductors is described, including sectioning and polishing protocols, optical microscopy, X-ray diffraction, scanning electron microscopy, optical spectroscopy, particle-induced X-ram emission, Rutherford backscattering, and electrical testing. Then collaboration with the University of Illinois at Urbana-Champaign is discussed in the areas of Hall-effect measurements and current voltage data. Finally, we discuss the strategy for continuing the program

Fiscal Year 2006

We describe progress in the development of new materials for portable, room-temperature, gamma-radiation detection at Pacific Northwest National Laboratory at the Hanford Site in Washington State. High Z, high resistivity, amorphous semiconductors are being designed for use as solid-state detectors at near ambient temperatures; principles of operation are analogous to single-crystal semiconducting detectors. Amorphous semiconductors have both advantages and disadvantages compared to single crystals, and this project is developing methods to mitigate technical problems and design optimized material for gamma detection. Several issues involved in the fabrication of amorphous semiconductors are described, including reaction thermodynamics and kinetics, the development of pyrolytic coating, and the synthesis of ingots. The characterization of amorphous semiconductors is described, including sectioning and polishing protocols, optical microscopy, X-ray diffraction, scanning electron microscopy, optical spectroscopy, particle-induced X-ram emission, Rutherford backscattering, and electrical testing. Then collaboration with the University of Illinois at Urbana-Champaign is discussed in the areas of Hall-effect measurements and current voltage data. Finally, we discuss the strategy for continuing the program

Materials Degradation and Detection (MD2): Deep Dive Final Report

An effort is underway at Pacific Northwest National Laboratory (PNNL) to develop a fundamental and general framework to foster the science and technology needed to support real-time monitoring of early degradation in materials used in the production of nuclear power. The development of such a capability would represent a timely solution to the mounting issues operators face with materials degradation in nuclear power plants. The envisioned framework consists of three primary and interconnected “thrust” areas including 1) microstructural science, 2) behavior assessment, and 3) monitoring and predictive capabilities. A brief state-of-the-art assessment for each of these core technology areas is discussed in the paper

Effects of Quartz Particle Size and Sucrose Addition on Melting Behavior of a Melter Feed for High-Level Glass

The behavior of melter feed (a mixture of nuclear waste and glass-forming additives) during waste-glass processing has a significant impact on the rate of the vitrification process. We studied the effects of silica particle size and sucrose addition on the volumetric expansion (foaming) of a high-alumina feed and the rate of dissolution of silica particles in feed samples heated at 5 C/min up to 1200 C. The initial size of quartz particles in feed ranged from 5 to 195 {micro}m. The fraction of the sucrose added ranged from 0 to 0.20 g per g glass. Extensive foaming occurred only in feeds with 5-{micro}m quartz particles; particles {ge}150 {micro}m formed clusters. Particles of 5 {micro}m completely dissolved by 900 C whereas particles {ge}150 {micro}m did not fully dissolve even when the temperature reached 1200 C. Sucrose addition had virtually zero impact on both foaming and the dissolution of silica particles. Over 100 sites in the United States are currently tasked with the storage of nuclear waste. The largest is the Hanford Site located in southeastern Washington State with 177 subterranean tanks containing over fifty-million gallons of nuclear waste from plutonium production from 1944 through 1987. This waste will be vitrified at the Hanford Tank Waste Treatment and Immobilization Plant. In the vitrification process, feed is charged into a melter and converted into glass to be ultimately stored in a permanent repository. The duration of waste-site cleanups by the vitrification process depends on the rate of melting, i.e., on the rate of the feed-to-glass conversion. Foaming associated with the melting process and the rate of dissolution of quartz particles (silica being the major glass-forming additive) are assumed to be important factors that influence the rate of melting. Previous studies on foaming of high-alumina feed demonstrated that varying the makeup of a melter feed has a significant impact on foaming. The volume of feeds that contained 5-{micro}m quartz particles substantially increased because of foaming. The extent of foaming decreased as the particle size of quartz increased. Moreover, samples containing quartz particles 195 {micro}m formed agglomerates at temperatures above 900 C that only slowly dissolved in the melt. This study continues previous work on the feed-melting process, specifically on the effects of the size of silica particles on the formation of nuclear-waste glasses to determine a suitable range of silica particle sizes that causes neither excessive foaming nor undesirable agglomeration. Apart from varying the silica-particle size, carbon was added in the form of sucrose. Sucrose has been used to accelerate the rate of melting. In this study, we have observed its impact on feed foaming and quartz dissolution