Chlorination of zirconium (0001) surface: A first-principles study.

Program Document · Sat Dec 31 23:00:00 EST 2016

OSTI ID:1429622

Kim, Eunja ^[1]; Weck, Philippe F ^[2]; Borjas, Rosendo ^[3]; Poineau, Frederic ^[3]

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1. Univ. of Nevada, Las Vegas, NV (United States). Dept. of Physics and Astronomy
2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
3. Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry

Here, the mechanisms and energetics of Zr(0001) surface chlorination by dissociative adsorption of gaseous Cl₂, and associated speciation and surface degradation processes, have been investigated within the framework of density functional theory. Chlorination of Zr(0001) is predicted to be exothermic by ~3 eV/Cl for dissociative adsorption of a single Cl₂ molecule, followed by exothermic chlorination to 1ML and 2 ML under Cl-rich conditions, with respective energy gains of 1.93 and 2.79 eV/Cl. Calculations also show that exfoliation of the top Cl-Zr-Cl sandwich layers is exothermic and most energetically favorable, and can thus be considered as a leading mechanism for Zr(0001) surface dissolution. Consistent with experimental findings, formation of ZrCl₄ molecular products is also found to be dominant during Zr(0001) chlorination.

• Research Organization: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
• Sponsoring Organization: USDOE Office of Nuclear Energy (NE)
• DOE Contract Number: AC04-94AL85000
• OSTI ID: 1429622
• Report Number(s): SAND2017--0774J; 650700
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY