Joseph Giaquinto

Application of ICP-MS radionuclide analysis to “Real World” samples of department of Energy radioactive waste

Disposal of Department of Energy (DOE) radioactive waste into repositories such as the Waste Isolation Pilot Plant (WIPP) and the Nevada Test Site (NTS) requires characterization to ensure regulatory and transportation requirements are met and to collect information regarding chemistry of the waste for processing concerns. Recent addition of an inductively coupled plasma quadrupole mass spectrometer in a radioactive contaminated laboratory at the Oak Ridge National Laboratory (ORNL) has allowed the evaluation of advantages of using ICP-MS over traditional techniques for some of these characterization needs. The measurement of long-lived beta nuclides (i.e.99Tc) by ICP-MS has resulted in improved detection limits and accuracy than the traditional counting techniques as well as reducing the need for separation/purification techniques which increase personnel exposure to radiation. Using ICP-MS for the measurement of U isotopes versus the traditional Thermal Ionization Mass Spectrometer (TIMS) technique has reduced cost and time by more than half while still maintaining the needed accuracy to determine risk assessment of the waste tanks. In addition, the application of ICP-MS to ORNL waste tank characterization has provided the opportunity to estimate non-routine radionuclides (i.e.135Cs and151Sm) and non-routine metals (i.e. Li, Ti, rare earths, etc.) using a rapid low cost screening method. These application methodologies and proficiencies on ORNL waste samples are summarized throughout the paper.

Inductively coupled plasma mass spectrometer installation modifications in a radioactive contaminated laboratory for the analysis of DOE radioactive waste streams

The operation and maintenance of a complex analytical instrument such as an inductively coupled plasma mass spectrometer in a radioactive contaminated environment presents unique problems and challenges that have to be considered in the purchasing and installation process. Considerations such as vendor experience, typical radiation levels, sample matrices encountered during sample analysis, instrument accessability for maintenance, and upkeep must be incorporated into the decision process. The Radioactive Materials Analytical Laboratory (RMAL) at Oak Ridge National Laboratory (ORNL) recently purchased and installed an inductively coupled plasma mass spectrometer for the analysis of Department of Energy (DOE) radioactive waste streams. This presentation will outline the purchasing decision, installation of the instrument, and how the modifications needed to operate in a radioactive contaminated laboratory do not significantly impact the daily operation and maintenance requirements of the instrument. Also, a contamination survey of the system will be presented which demonstrates the contamination levels in the instrument from the sample introduction system to the detector.

Integration of a hyphenated HPIC-ICPMS protocol for the measurement of transplutonium isotopic mass distributions for 252Cf campaigns at Oak Ridge National Laboratory

Rapid measurement of transplutonium isotopic mass distributions during 252Cf production campaigns at Oak Ridge National Laboratory is a critical need. Mass measurements for the isotopes of plutonium, americium, curium, and californium are routinely requested to support the α-hydroxy-isobutyrate runs for the purification and recovery of the heavy curium target material and final 249Bk, 252Cf, and 254Es enriched isotope products. This paper presents the integration of an online high-pressure ion chromatography inductively coupled plasma mass spectrometry technique together with the protocol and chemistry that allows for rapid baseline separation and direct quantification of the transplutonium elemental concentrations and isotopic compositions.

Trace impurity analysis in uranium oxide via hybrid quantification techniques—gravimetric standard addition and isotope dilution mass spectrometry

Measurement methods for the analysis of trace impurities in uranium materials, essential in nuclear fuel production and nuclear forensics, are continuously improving. Analytical methods were developed with the goal of lowering uncertainties of next generation certified uranium oxide reference materials for trace impurity concentrations. Through addition of a traceable standard directly into the sample, gravimetric standard addition and isotope dilution followed by analysis on an inductively coupled plasma mass spectrometer can achieve lower uncertainties. Results for 28 impurities in CRM 124-1 and 124-6 from NBL Program Office were used for validation of accuracy and comparisons of uncertainties.

Milestone report - M4FT-14OR0302102b - Evaluation of Tritium Content and Release from Surry-2 Fuel Cladding

To design and operate future reprocessing plants in a safe and environmentally compliant manner, the amount and form of tritium in the used nuclear fuel (UNF) must be understood and quantified.To gain a better understanding of how tritium in cladding will behave during processing, scoping tests are being performed to determine the tritium content in the cladding pre- and post-tritium pretreatment. A sample of Surry-2 pressurized water reactor (PWR) cladding was heated to 1100–1200°C to oxidize the zirconium and release all of the tritium in the cladding sample. The tritium content was measured to be ~240 µCi/g. Cladding samples were heated to 500oC, which is within the temperature range (480 - 600oC) expected for standard air tritium pretreatment systems, and to a slightly higher temperature (700oC) to determine the impact of tritium pretreatment on tritium release from the cladding. Heating at 500°C for 24 hr removes ~0.2% of the tritium from the cladding, and heating at 700°C for 24 hr removes ~9%. Thus, a significant fraction of the tritium remains bound in the cladding and must be considered in operations involving cladding recycle.