Helium interactions with alumina formed by atomic layer deposition show potential for mitigating problems with excess helium in spent nuclear fuel

Zhang, Shenli; Yu, Erick; Gates, Sean; Cassata, William S.; Makel, James; Thron, Andrew M.; Bartel, Christopher; Weimer, Alan W.; Faller, Roland; Stroeve, Pieter; Tringe, Joseph W.

doi:10.1016/j.jnucmat.2017.11.029

Title: Helium interactions with alumina formed by atomic layer deposition show potential for mitigating problems with excess helium in spent nuclear fuel

Journal Article · Sun Nov 26 00:00:00 EST 2017 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2017.11.029· OSTI ID:1476185

Zhang, Shenli ^[1]; Yu, Erick ^[1]; Gates, Sean ^[2]; Cassata, William S. ^[2]; Makel, James ^[3]; Thron, Andrew M. ^[1]; Bartel, Christopher ^[4]; Weimer, Alan W. ^[4]; Faller, Roland ^[3]; Stroeve, Pieter ^[3]; Tringe, Joseph W. ^[2]

Univ. of California, Davis, CA (United States). Dept. of Materials Science and Engineering
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Univ. of California, Davis, CA (United States). Dept. of Chemical Engineering
Univ. of Colorado, Boulder, CO (United States). Dept. of Chemical and Biological Engineering

Helium gas accumulation from alpha decay during extended storage of spent fuel has potential to compromise the structural integrity the fuel. We report results obtained with surrogate nickel particles which suggest that alumina formed by atomic layer deposition can serve as a low volume-fraction, uniformly-distributed phase for retention of helium generated in fuel particles such as uranium oxide. Thin alumina layers may also form transport paths for helium in the fuel rod, which would otherwise be impermeable. Micron-scale nickel particles, representative of uranium oxide particles in their low helium solubility and compatibility with the alumina synthesis process, were homogeneously coated with alumina approximately 3–20 nm by particle atomic layer deposition (ALD) using a fluidized bed reactor. Particles were then loaded with helium at 800 °C in a tube furnace. Subsequent helium spectroscopy measurements showed that the alumina phase, or more likely a related nickel/alumina interface structure, retains helium at a density of at least 10¹⁷ atoms/cm³. High resolution transmission electron microscopy revealed that the thermal treatment increased the alumina thickness and generated additional porosity. Results from Monte Carlo simulations on amorphous alumina predict the helium retention concentration at room temperature could reach 10²¹ atoms/cm³ at 400 MPa, a pressure predicted by others to be developed in uranium oxide without an alumina secondary phase. This concentration is sufficient to eliminate bubble formation in the nuclear fuel for long-term storage scenarios, for example. Finally, measurements by others of the diffusion coefficient in polycrystalline alumina indicate values several orders of magnitude higher than in uranium oxide, which then can also allow for helium transport out of the spent fuel.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Univ. of California, Davis, CA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC52-07NA27344; NE0000704; DE–NE0000704

OSTI ID:: 1476185

Alternate ID(s):: OSTI ID: 1549135

Report Number(s):: LLNL-JRNL-743180; 886825

Journal Information:: Journal of Nuclear Materials, Vol. 499; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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Liquid fuel synthesis in microreactors Hafeez, Sanaa; Manos, George; Al-Salem, S. M. Reaction Chemistry & Engineering, Vol. 3, Issue 4 https://doi.org/10.1039/c8re00040a	journal	January 2018
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