Understanding Structure and Stability of Monoclinic Zirconia Surfaces from First-Principles Calculations
Bazhenov, A., & Honkala, K. (2017). Understanding Structure and Stability of Monoclinic Zirconia Surfaces from First-Principles Calculations. Topics in Catalysis, 60(6), 382-391. https://doi.org/10.1007/s11244-016-0701-0
Julkaistu sarjassa
Topics in CatalysisPäivämäärä
2017Tekijänoikeudet
© Springer Science+Business Media New York 2016. This is a final draft version of an article whose final and definitive form has been published by Springer. Published in this repository with the kind permission of the publisher.
Under the water-rich pre-treatment and/or reaction
conditions, structure and chemistry of the monoclinic
zirconia surfaces are strongly influenced by oxygen vacancies
and incorporated water. Here, we report a combined
first-principles and atomistic thermodynamics study on the
structure and stability of selected surfaces of the monoclinic
zirconia. Our results indicate that among the studied surfaces,
the most stable (111) surface is the least vulnerable
towards oxygen vacancies in contrast to the less stable (011)
and (101) surfaces, where formation of oxygen vacancies
is energetically more favorable. Furthermore, we present a
vigorous, systematic screening of water incorporation onto
the studied surfaces. We observe that the greatest stabilization
of the surfaces is achieved when a part of the adsorbed
water molecules is dissociated. Nevertheless, the importance
of water dissociation for achieving the greatest stabilization
is high for the less stable (011) and (101) surfaces, while
completely hydrated (111) surface is stabilized equally regardless
of the water dissociation state. Analysis of the constructed
phase diagrams reveals that the (111) surface remains
preferably clean and the (011) and (101) surfaces have
dissociated water at low coverage under the reactive conditions
of T = 600–900 K and p(H2O) < 1 bar. Upon temperature
decrease and/or pressure increase, all studied surfaces
gradually uptake water until fully hydrated. All in all, our
findings complement and broaden the existing picture of the
structure and stability of the monoclinic zirconia surfaces
under the pre-treatment and/or reaction conditions, enabling
rationalization of the potential roles of zirconia as a heterogeneous
support and a catalyst component.
...
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