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Structural and Chemical Transformations of Zinc Oxide Ultrathin Films on Pd(111) Surfaces. | LitMetric

Structural and Chemical Transformations of Zinc Oxide Ultrathin Films on Pd(111) Surfaces.

ACS Appl Mater Interfaces

Davidson School of Chemical Engineering, Purdue University, 480 Stadium Mall Drive, West Lafayette, Indiana 47906, United States.

Published: July 2021

AI Article Synopsis

Article Abstract

Structural and chemical transformations of ultrathin oxide films on transition metals lie at the heart of many complex phenomena in heterogeneous catalysis, such as the strong metal-support interaction (SMSI). However, there is limited atomic-scale understanding of these transformations, especially for irreducible oxides such as ZnO. Here, by combining density functional theory calculations and surface science techniques, including scanning tunneling microscopy, X-ray photoelectron spectroscopy, high-resolution electron energy loss spectroscopy, and low-energy electron diffraction, we investigated the interfacial interaction of well-defined ultrathin ZnOH films on Pd(111) under varying gas-phase conditions [ultrahigh vacuum (UHV), 5 × 10 mbar of O, and a D/O mixture] to shed light on the SMSI effect of irreducible oxides. Sequential treatment of submonolayer zinc oxide films in a D/O mixture (1:4) at 550 K evoked reversible structural transformations from a bilayer to a monolayer and further to a Pd-Zn near-surface alloy, demonstrating that zinc oxide, as an irreducible oxide, can spread on metal surfaces and show an SMSI-like behavior in the presence of hydrogen. A mixed canonical-grand canonical phase diagram was developed to bridge the gap between UHV conditions and true SMSI environments, revealing that, in addition to surface alloy formation, certain ZnOH films with stoichiometries that do not exist in bulk are stabilized by Pd in the presence of hydrogen. Based on the combined theoretical and experimental observations, we propose that SMSI metal nanoparticle encapsulation for irreducible oxide supports such as ZnO involves both surface (hydroxy)oxide and surface alloy formation, depending on the environmental conditions.

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Source
http://dx.doi.org/10.1021/acsami.1c07510DOI Listing

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