Airborne Release Fractions from Surrogate Nuclear Waste Fires Containing Lanthanide Nitrates and Depleted Uranium Nitrate in 30% Tributyl Phosphate in Kerosene

Abstract

Airborne contaminants from fires containing nuclear waste represent significant health hazards and shape the design and operation of nuclear facilities. Much of the data used to formulate DOE-HDBK-3010-94, “Airborne Release Fractions/Rates and Respirable Fractions for Nonreactor Nuclear Facilities,” from the U.S. Department of Energy, were taken over 40 years ago. The objectives of this study were to reproduce experiments from Pacific Northwest Laboratories conducted in June 1973 employing current aerosol measurement methods and instrumentation, develop an enhanced understanding of particulate formation and transport from fires containing nuclear waste, and provide modeling and experimental capabilities for updating current standards and practices in nuclear facilities. A special chamber was designed to conduct small fires containing 25 mL of flammable waste containing lutetium nitrate, ytterbium nitrate, or depleted uranium nitrate. Carbon soot aerosols showed aggregates of primary particles ranging from 20 to 60 nm in diameter. In scanning electron microscopy, ~200-nm spheroidal particles were also observed dispersed among the fractal aggregates. The 200-nm spherical particles were composed of metal phosphates. Airborne release fractions (ARFs) were characterized by leaching filter deposits and quantifying metal concentrations with mass spectrometry. The average mass-based ARF for ²³⁸U experiments was 1.0 × 10⁻³ with a standard deviation of 7.5 × 10⁻⁴. For the original experiments, DOE-HDBK-3010-94 states, “Uranium ARFs range from 2 × 10⁻⁴ to 3 × 10⁻³, an uncertainty of approximately an order of magnitude.” Thus, current measurements were consistent with DOE-HDBK-3010-94 values. ARF values for lutetium and ytterbium were approximately one to two orders of magnitude lower than ²³⁸U. Metal nitrate solubility may have varied with elemental composition and temperature, thereby affecting ARF values for uranium surrogates (Yb and Lu). In addition to ARF data, solution boiling temperatures and evaporation rates can also be deduced from experimental data.

Keywords:

• Airborne release fraction
• kerosene
• tributyl phosphate
• fire
• DOE-HDBK-3010-94

Acknowledgments

This work was funded by the Nuclear Safety Research and Development Program, which is managed by the Office of Nuclear Safety, within the Office of Environment, Health, Safety and Security to provide corporate-level leadership supporting nuclear safety research and development throughout the DOE. SNL is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the DOE’s National Nuclear Security Administration under contract DE-NA0003525.