Abstract
The characterization of zirconium hydride is important in the nuclear industry because of the hydrogen-induced embrittlement of Zircaloy cladding and its use as a neutron moderator. This paper introduces the use of Raman spectroscopy for the characterization of zirconium hydride. First-principles density functional theory (DFT) calculations were used to predict the Raman spectra of ζ-ZrH0.5, γ-ZrH, δ-ZrH1.5, δ-ZrH1.66, and ε-ZrH2 with all their predicted symmetries; ζ-ZrH0.5 (P3m1, R3¯m, C2/m, Cm, Cmmm, and Pn3¯m); γ-ZrH (P222, Ccce, and P42/mmc); δ-ZrH1.5 (P4¯m2, P42/mcm, Fmmm, Pn3¯m, Ibam, P2/c, PI, and P42/nnm); δ-ZrH1.66 (Fm3¯m); and ε-ZrH2 (Fm3¯m, R3¯m, and I4/mmm). Two samples of Zircaloy-4 containing 133 wt ppm and 360 wt ppm hydrogen were characterized by Raman spectroscopy, showing two signal lines at 215 cm−1 and 1,187 cm−1, which were assigned to the presence of δ-ZrH1.66. These signals had a good spatial correlation with visible hydride precipitates in Raman spectroscopy images. This work provides the basis for the characterization of all possible zirconium hydride compositions and structures using Raman spectroscopy.
| Original language | English |
|---|---|
| Article number | 154988 |
| Journal | Journal of Nuclear Materials |
| Volume | 593 |
| DOIs | |
| State | Published - May 2024 |
Funding
This work was sponsored by the US Department of Energy (DOE) Office of Nuclear Energy's Advanced Fuels Campaign. Portions of this work were sponsored by the DOE National Nuclear Security Administration Office of Defense Nuclear Nonproliferation. Theoretical calculations research was supported by the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility at Oak Ridge National Laboratory. This research used resources of the National Energy Research Scientific Computing Center , which is a DOE Office of Science User Facility operated under Contract No. DE-AC02-05CH11231 . Authors would like to acknowledge Andrew Nelson for the insightful discussions on the use of Raman spectroscopy. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).This work was sponsored by the US Department of Energy (DOE) Office of Nuclear Energy's Advanced Fuels Campaign. Portions of this work were sponsored by the DOE National Nuclear Security Administration Office of Defense Nuclear Nonproliferation. Theoretical calculations research was supported by the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility at Oak Ridge National Laboratory. This research used resources of the National Energy Research Scientific Computing Center, which is a DOE Office of Science User Facility operated under Contract No. DE-AC02-05CH11231. Authors would like to acknowledge Andrew Nelson for the insightful discussions on the use of Raman spectroscopy.
| Funders | Funder number |
|---|---|
| Center for Nanophase Materials Sciences | |
| DOE National Nuclear Security Administration Office of Defense Nuclear Nonproliferation | |
| DOE Public Access Plan | |
| U.S. Department of Energy | |
| Office of Science | |
| Oak Ridge National Laboratory | DE-AC02-05CH11231 |
Keywords
- DFT calculations
- Raman spectroscopy
- Zirconium hydride