Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy

Reinecke, Benjamin N.; Kuhl, Kendra P.; Ogasawara, Hirohito; Li, Lin; Voss, Johannes; Abild-Pedersen, Frank; Nilsson, Anders; Jaramillo, Thomas F.

doi:10.1016/j.susc.2015.12.025

Title: Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy

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Abstract

We report on the electronic structure of Au (gold) nanoparticles supported onto TiO₂ with a goal of elucidating the most important effects that contribute to their high catalytic activity. We synthesize and characterize with high resolution transmission electron microscopy (HRTEM) 3.4, 5.3, and 9.5 nm diameter TiO₂-supported Au nanoparticles with nearly spherical shape and measure their valence band using Au 5d subshell sensitive hard X-ray photoelectron spectroscopy (HAXPES) conducted at Spring-8. Based on density functional theory (DFT) calculations of various Au surface structures, we interpret the observed changes in the Au 5d valence band structure as a function of size in terms of an increasing percentage of Au atoms at corners/edges for decreasing particle size. Finally, this work elucidates how Au coordination number impacts the electronic structure of Au nanoparticles, ultimately giving rise to their well-known catalytic activity.

Authors:

Reinecke, Benjamin N. ^[1]; Kuhl, Kendra P. ^[1]; Ogasawara, Hirohito ^[2]; Li, Lin ^[1]; Voss, Johannes ^[2]; Abild-Pedersen, Frank ^[2]; Nilsson, Anders ^[2]; Jaramillo, Thomas F. ^[3]

Stanford Univ., Stanford, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: Thu Dec 31 00:00:00 EST 2015

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

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

OSTI Identifier:: 1351302

Alternate Identifier(s):: OSTI ID: 1434058

Grant/Contract Number:: 1066515; ECS-9731293; AC02-76SF00515; 2009B1751

Resource Type:: Accepted Manuscript

Journal Name:: Surface Science

Additional Journal Information:: Journal Volume: 650; 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; 36 MATERIALS SCIENCE; gold nanoparticles; transmission electron microscopy; valence band; support effect; titanium dioxide; hard X-ray photoelectron spectroscopy

Citation Formats


                    Reinecke, Benjamin N., Kuhl, Kendra P., Ogasawara, Hirohito, Li, Lin, Voss, Johannes, Abild-Pedersen, Frank, Nilsson, Anders, and Jaramillo, Thomas F. Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy.  United States: N. p., 2015. 
Web.  doi:10.1016/j.susc.2015.12.025.

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                    Reinecke, Benjamin N., Kuhl, Kendra P., Ogasawara, Hirohito, Li, Lin, Voss, Johannes, Abild-Pedersen, Frank, Nilsson, Anders, & Jaramillo, Thomas F. Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy.  United States.  https://doi.org/10.1016/j.susc.2015.12.025

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                    Reinecke, Benjamin N., Kuhl, Kendra P., Ogasawara, Hirohito, Li, Lin, Voss, Johannes, Abild-Pedersen, Frank, Nilsson, Anders, and Jaramillo, Thomas F. Thu .  
"Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy".  United States.  https://doi.org/10.1016/j.susc.2015.12.025.  https://www.osti.gov/servlets/purl/1351302.

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@article{osti_1351302,

  title        = {Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy},

  author       = {Reinecke, Benjamin N. and Kuhl, Kendra P. and Ogasawara, Hirohito and Li, Lin and Voss, Johannes and Abild-Pedersen, Frank and Nilsson, Anders and Jaramillo, Thomas F.},

  abstractNote = {We report on the electronic structure of Au (gold) nanoparticles supported onto TiO2 with a goal of elucidating the most important effects that contribute to their high catalytic activity. We synthesize and characterize with high resolution transmission electron microscopy (HRTEM) 3.4, 5.3, and 9.5 nm diameter TiO2-supported Au nanoparticles with nearly spherical shape and measure their valence band using Au 5d subshell sensitive hard X-ray photoelectron spectroscopy (HAXPES) conducted at Spring-8. Based on density functional theory (DFT) calculations of various Au surface structures, we interpret the observed changes in the Au 5d valence band structure as a function of size in terms of an increasing percentage of Au atoms at corners/edges for decreasing particle size. Finally, this work elucidates how Au coordination number impacts the electronic structure of Au nanoparticles, ultimately giving rise to their well-known catalytic activity.},

  doi          = {10.1016/j.susc.2015.12.025},

  journal      = {Surface Science},

  number       = C,

  volume       = 650,

  place        = {United States},

  year         = {Thu Dec 31 00:00:00 EST 2015},

  month        = {Thu Dec 31 00:00:00 EST 2015}

}

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