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Title: Non-equilibrium oxidation states of zirconium during early stages of metal oxidation

Journal Article · · Applied Physics Letters
DOI:https://doi.org/10.1063/1.4914180· OSTI ID:22395696
;  [1];  [1];  [2]
  1. Laboratory for Electrochemical Interfaces, Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139 (United States)
  2. Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973 (United States)

The chemical state of Zr during the initial, self-limiting stage of oxidation on single crystal zirconium (0001), with oxide thickness on the order of 1 nm, was probed by synchrotron x-ray photoelectron spectroscopy. Quantitative analysis of the Zr 3d spectrum by the spectrum reconstruction method demonstrated the formation of Zr{sup 1+}, Zr{sup 2+}, and Zr{sup 3+} as non-equilibrium oxidation states, in addition to Zr{sup 4+} in the stoichiometric ZrO{sub 2}. This finding resolves the long-debated question of whether it is possible to form any valence states between Zr{sup 0} and Zr{sup 4+} at the metal-oxide interface. The presence of local strong electric fields and the minimization of interfacial energy are assessed and demonstrated as mechanisms that can drive the formation of these non-equilibrium valence states of Zr.

OSTI ID:
22395696
Journal Information:
Applied Physics Letters, Vol. 106, Issue 10; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0003-6951
Country of Publication:
United States
Language:
English

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Zirconium carbide oxidation: Kinetics and oxygen diffusion through the intermediate layer journal February 2018
DC electrical degradation of YSZ: Voltage‐controlled electrical metallization of a fast ion conducting insulator journal January 2020
The Initial Stage in Oxidation of ZrNiSn (Half Heusler) Alloy by Oxygen journal May 2019