Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces

Zhu, Yaguang; Wu, Dongxiang; Liu, Qianqian; Sadowski, Jerzy T.; Zhou, Guangwen

doi:10.1021/acs.jpcc.9b00750

Title: Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces

Abstract

Nearly, all metals form spontaneously an oxygenated surface upon exposure to air. We demonstrate that the reaction of such an oxygenated surface with hydrogen results in the clustering of metal atoms. Using scanning electron microcopy, X-ray photoelectron spectroscopy, and in situ low-energy electron microscopy, we show that Cu atoms in the oxygenated Cu(110) surface self-assemble into Cu clusters upon the hydrogen-induced loss of the chemisorbed oxygen. It is shown that the clustering of Cu atoms occurs preferentially along the upper side of step edges formed by neighboring terraces of the substrate and boundaries of heterophase domains on the same terrace, followed by the spreading across the entire surface as the reaction progresses toward completion. Using density functional theory calculations, we show that the heterogeneous clustering of Cu atoms is induced by step-crossing barriers that hinder Cu atoms crossing descendent steps, thereby resulting in three-dimensional aggregation of Cu atoms on the upper side of step edges. These results may find broader applicability to tailor the formation of metal clusters for elucidating the intrinsic properties and functionalities of nanoclusters.

Authors:

Zhu, Yaguang ^[1]; Wu, Dongxiang ^[1]; Liu, Qianqian ^[1]; Sadowski, Jerzy T. ^[2];

^[1]

State Univ. of New York (SUNY), Binghamton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials

Publication Date:: Thu Apr 18 00:00:00 EDT 2019

Research Org.:: Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); State Univ. of New York (SUNY), Binghamton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Binghamton Univ., NY (United States)

Sponsoring Org.:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1514384

Alternate Identifier(s):: OSTI ID: 1594001; OSTI ID: 1864745

Report Number(s):: BNL-211643-2019-JAAM
Journal ID: ISSN 1932-7447

Grant/Contract Number:: SC0012704; SC0001135; AC02-06CH11357; OCI-1053575

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 123; Journal Issue: 18; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Cu(110); oxidation; STM; LEEM; O2; H2

Citation Formats


                    Zhu, Yaguang, Wu, Dongxiang, Liu, Qianqian, Sadowski, Jerzy T., and Zhou, Guangwen. Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces.  United States: N. p., 2019. 
Web.  doi:10.1021/acs.jpcc.9b00750.

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                    Zhu, Yaguang, Wu, Dongxiang, Liu, Qianqian, Sadowski, Jerzy T., & Zhou, Guangwen. Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces.  United States.  https://doi.org/10.1021/acs.jpcc.9b00750

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                    Zhu, Yaguang, Wu, Dongxiang, Liu, Qianqian, Sadowski, Jerzy T., and Zhou, Guangwen. Thu .  
"Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces".  United States.  https://doi.org/10.1021/acs.jpcc.9b00750.  https://www.osti.gov/servlets/purl/1514384.

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@article{osti_1514384,

  title        = {Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces},

  author       = {Zhu, Yaguang and Wu, Dongxiang and Liu, Qianqian and Sadowski, Jerzy T. and Zhou, Guangwen},

  abstractNote = {Nearly, all metals form spontaneously an oxygenated surface upon exposure to air. We demonstrate that the reaction of such an oxygenated surface with hydrogen results in the clustering of metal atoms. Using scanning electron microcopy, X-ray photoelectron spectroscopy, and in situ low-energy electron microscopy, we show that Cu atoms in the oxygenated Cu(110) surface self-assemble into Cu clusters upon the hydrogen-induced loss of the chemisorbed oxygen. It is shown that the clustering of Cu atoms occurs preferentially along the upper side of step edges formed by neighboring terraces of the substrate and boundaries of heterophase domains on the same terrace, followed by the spreading across the entire surface as the reaction progresses toward completion. Using density functional theory calculations, we show that the heterogeneous clustering of Cu atoms is induced by step-crossing barriers that hinder Cu atoms crossing descendent steps, thereby resulting in three-dimensional aggregation of Cu atoms on the upper side of step edges. These results may find broader applicability to tailor the formation of metal clusters for elucidating the intrinsic properties and functionalities of nanoclusters.},

  doi          = {10.1021/acs.jpcc.9b00750},

  journal      = {Journal of Physical Chemistry. C},

  number       = 18,

  volume       = 123,

  place        = {United States},

  year         = {Thu Apr 18 00:00:00 EDT 2019},

  month        = {Thu Apr 18 00:00:00 EDT 2019}

}

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Title: Hydrogen-Induced Clustering of Metal Atoms in Oxygenated Metal Surfaces

Abstract

Citation Formats

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Kinetic Barriers of the Phase Transition in the Oxygen Chemisorbed Cu(110)-(2 × 1)-O as a Function of Oxygen Coverage journal, August 2014

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Strain engineering tunable nanotemplates on the Cu(110)–(2×1)–O surface journal, October 2010

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