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Title: Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface

Abstract

Weak inter-adsorbate interactions are shown to play a crucial role in determining surface structure, with major implications for its catalytic reactivity. This is exemplified here in the case of acetate bound to Au(110), where the small extra energy of the van der Waals interactions among the surface-bound groups drives massive restructuring of the underlying Au. Acetate is a key intermediate in electro-oxidation of CO 2 and a poison in partial oxidation reactions. Metal atom migration originates at surface defects and is likely facilitated by weakened Au–Au interactions due to bonding with the acetate. Even though the acetate is a relatively small molecule, weak intermolecular interaction provides the energy required for molecular self-assembly and reorganization of the metal surface.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [3];  [4];  [5]
  1. Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
  2. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Science. Dept. of Physics; Univ. of Science and Technology of China, Hefei (China). Synergetic Innovation Center of Quantum Information and Quantum Physics. Hefei National Lab. for Physical Sciences at Microscale. International Center for Quantum Design of Functional Materials (ICQD)
  3. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Science
  4. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Science. Dept. of Physics
  5. Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology. School of Engineering and Applied Science
Publication Date:
Research Org.:
Oak Ridge National Laboratory, Oak Ridge Leadership Computing Facility (OLCF); Harvard Univ., Cambridge, MA (United States); Univ. of Science and Technology of China, Hefei (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1362265
Grant/Contract Number:  
SC0012573; 11504357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalysis; Imaging techniques; Surface assembly; Theory and computation

Citation Formats

Hiebel, Fanny, Shong, Bonggeun, Chen, Wei, Madix, Robert J., Kaxiras, Efthimios, and Friend, Cynthia M. Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface. United States: N. p., 2016. Web. doi:10.1038/ncomms13139.
Hiebel, Fanny, Shong, Bonggeun, Chen, Wei, Madix, Robert J., Kaxiras, Efthimios, & Friend, Cynthia M. Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface. United States. doi:10.1038/ncomms13139.
Hiebel, Fanny, Shong, Bonggeun, Chen, Wei, Madix, Robert J., Kaxiras, Efthimios, and Friend, Cynthia M. Wed . "Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface". United States. doi:10.1038/ncomms13139. https://www.osti.gov/servlets/purl/1362265.
@article{osti_1362265,
title = {Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface},
author = {Hiebel, Fanny and Shong, Bonggeun and Chen, Wei and Madix, Robert J. and Kaxiras, Efthimios and Friend, Cynthia M.},
abstractNote = {Weak inter-adsorbate interactions are shown to play a crucial role in determining surface structure, with major implications for its catalytic reactivity. This is exemplified here in the case of acetate bound to Au(110), where the small extra energy of the van der Waals interactions among the surface-bound groups drives massive restructuring of the underlying Au. Acetate is a key intermediate in electro-oxidation of CO2 and a poison in partial oxidation reactions. Metal atom migration originates at surface defects and is likely facilitated by weakened Au–Au interactions due to bonding with the acetate. Even though the acetate is a relatively small molecule, weak intermolecular interaction provides the energy required for molecular self-assembly and reorganization of the metal surface.},
doi = {10.1038/ncomms13139},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {10}
}

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Works referenced in this record:

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865