Oxygen adsorption on spontaneously reconstructed Au(511)

Xu, Fang; Montemore, Matthew M.; O'Connor, Christopher R.; Muramoto, Eri; van Spronsen, Matthijs A.; Madix, Robert J.; Friend, Cynthia M.

doi:10.1016/j.susc.2018.09.012

Title: Oxygen adsorption on spontaneously reconstructed Au(511)

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Abstract

The four-fold site on {100} facets, which are potential catalytic sites on high-curvature gold nanoparticles, is difficult to prepare on a gold single crystal due to surface reconstruction. In this work, the Au(511) surface with a high density of step edges and a well-maintained {100} local structure was studied by scanning tunneling microscopy (STM), temperature programmed reaction spectroscopy (TPRS), and density functional theory (DFT) calculations. Annealing at 550 K and 870 K induces reconstruction on the Au(511) surface to a mixture of (311) and (711) micro-terraces. At room temperature and low oxygen coverage, oxygen adsorbs at both three- and four-fold sites on the surface, leading to a well-ordered zig-zag structure. Oxygen atoms cause significant orbital hybridization and a slight displacement of the gold atoms to which they bind. High oxygen coverages induce the formation of clusters, which are not active towards oxidation of isopropanol at room temperature and a pressure of 10^-10 mbar. Oxygen adsorption saturates at 1 monolayer (ML), and two separate oxygen recombinative desorption peaks were observed at coverages above 0.11 ML. Our characterization of this surface and the O adsorption structure offers future studies of {100} micro-terraces for oxidation reactions, which contributes to studies on gold-based catalystsmore » with an irregular shape.« less

Authors:

Xu, Fang ^[1];

^[1]; O'Connor, Christopher R. ^[1]; Muramoto, Eri ^[1]; van Spronsen, Matthijs A. ^[1]; Madix, Robert J. ^[1]; Friend, Cynthia M. ^[1]

Harvard Univ., Cambridge, MA (United States)

Publication Date:: 2018-09-21

Research Org.:: Harvard Univ., Cambridge, MA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1597444

Alternate Identifier(s):: OSTI ID: 1636030

Grant/Contract Number:: SC0012573

Resource Type:: Accepted Manuscript

Journal Name:: Surface Science

Additional Journal Information:: Journal Volume: 679; Journal Issue: C; Journal ID: ISSN 0039-6028

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Gold surface; Oxygen desorption; Reconstruction; STM; DFT calculations

Citation Formats


                    Xu, Fang, Montemore, Matthew M., O'Connor, Christopher R., Muramoto, Eri, van Spronsen, Matthijs A., Madix, Robert J., and Friend, Cynthia M. Oxygen adsorption on spontaneously reconstructed Au(511).  United States: N. p., 2018. 
Web.  doi:10.1016/j.susc.2018.09.012.

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                    Xu, Fang, Montemore, Matthew M., O'Connor, Christopher R., Muramoto, Eri, van Spronsen, Matthijs A., Madix, Robert J., & Friend, Cynthia M. Oxygen adsorption on spontaneously reconstructed Au(511).  United States.  https://doi.org/10.1016/j.susc.2018.09.012

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                    Xu, Fang, Montemore, Matthew M., O'Connor, Christopher R., Muramoto, Eri, van Spronsen, Matthijs A., Madix, Robert J., and Friend, Cynthia M. Fri .  
"Oxygen adsorption on spontaneously reconstructed Au(511)".  United States.  https://doi.org/10.1016/j.susc.2018.09.012.  https://www.osti.gov/servlets/purl/1597444.

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@article{osti_1597444,

  title        = {Oxygen adsorption on spontaneously reconstructed Au(511)},

  author       = {Xu, Fang and Montemore, Matthew M. and O'Connor, Christopher R. and Muramoto, Eri and van Spronsen, Matthijs A. and Madix, Robert J. and Friend, Cynthia M.},

  abstractNote = {The four-fold site on {100} facets, which are potential catalytic sites on high-curvature gold nanoparticles, is difficult to prepare on a gold single crystal due to surface reconstruction. In this work, the Au(511) surface with a high density of step edges and a well-maintained {100} local structure was studied by scanning tunneling microscopy (STM), temperature programmed reaction spectroscopy (TPRS), and density functional theory (DFT) calculations. Annealing at 550 K and 870 K induces reconstruction on the Au(511) surface to a mixture of (311) and (711) micro-terraces. At room temperature and low oxygen coverage, oxygen adsorbs at both three- and four-fold sites on the surface, leading to a well-ordered zig-zag structure. Oxygen atoms cause significant orbital hybridization and a slight displacement of the gold atoms to which they bind. High oxygen coverages induce the formation of clusters, which are not active towards oxidation of isopropanol at room temperature and a pressure of 10-10 mbar. Oxygen adsorption saturates at 1 monolayer (ML), and two separate oxygen recombinative desorption peaks were observed at coverages above 0.11 ML. Our characterization of this surface and the O adsorption structure offers future studies of {100} micro-terraces for oxidation reactions, which contributes to studies on gold-based catalysts with an irregular shape.},

  doi          = {10.1016/j.susc.2018.09.012},

  journal      = {Surface Science},

  number       = C,

  volume       = 679,

  place        = {United States},

  year         = {2018},

  month        = {9}

}

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