Physical conditions for UO formation in laser-produced uranium plumes

Harilal, Sivanandan S.; Kautz, Elizabeth J.; Bernacki, Bruce E.; Phillips, Mark C.; Skrodzki, Patrick J.; Burger, Milos; Jovanovic, I

doi:10.1039/c9cp02250c

Physical conditions for UO formation in laser-produced uranium plumes

Journal Article · Wed Aug 07 00:00:00 EDT 2019 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c9cp02250c· OSTI ID:1568063

^[1]; Kautz, Elizabeth J. ^[1]; Bernacki, Bruce E. ^[1]; Phillips, Mark C. ^[2]; Skrodzki, Patrick J. ^[3]; Burger, Milos ^[3]; Jovanovic, I ^[4]

BATTELLE (PACIFIC NW LAB)
UNIVERSITY PROGRAMS
UNIVERSITY OF MICHIGAN
University of Michigan

We investigate the oxidation of uranium (U) species, the physical conditions leading to uranium monoxide (UO) formation, and the interplay between plume hydrodynamics and plasma chemistry in a laser-produced uranium plasma. The plasmas are produced by ablation of metallic U using nanosecond laser pulses. An ambient gas environment with varying oxygen partial pressures in 100 Torr inert Ar gas is used for controlling the plasma oxidation chemistry. Optical emission spectroscopic analysis of U atomic and monoxide species shows a reduction of the emission intensity and persistence with increasing oxygen partial pressure. Spectral modeling is used for identifying the physical conditions in the plasma that favor UO formation. The optimal temperature for UO formation is found to be in the temperature range of ~1500–5000 K. The spectrally-integrated and spectrally-filtered (monochromatic) imaging of U atomic and molecular species reveal the evolutionary paths of oxidation U species in the plasma. Our results also highlight that oxidation in U plasmas predominantly happens at the cooler plasma periphery, is delayed with respect to plasma formation, and the dissipation of molecular species strongly depends on oxygen partial pressure.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1568063

Report Number(s):: PNNL-SA--143238

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 29 Vol. 21

Country of Publication:: United States

Language:: English

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