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Title: Morphology and chemical behavior of model CsO x/Cu 2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO 2 and H 2

Abstract

Cs is a promoter of Cu-based catalysts for the synthesis of alcohols from CO 2 hydrogenation. Scanning tunneling microscopy and ambient-pressure x-ray photoelectron spectroscopy were used to study the morphology and chemical properties of surfaces generated by the deposition of cesium on Cu 2O/Cu(111) and Cu(111) substrates. CsO x nanostructures were formed after Cs metal was deposited on Cu 2O/Cu(111) at 300 K. The formed CsO x protrude over the surface of copper oxide by 2–4 Å, with the dimension at the base of the nanostructures being in the range of 1–3 nm. Heating to elevated temperature induced significant changes in the size and dispersion of the CsO x nanostructures, and there was a clear reconstruction of the copper oxide substrate, which then exhibited long range order with a hexagonally packed structure. The as-deposited and annealed surfaces of CsO x/Cu 2O/Cu(111) were more reactive toward CO 2 than plain Cu 2O/Cu(111) or clean Cu(111). Yet, none of them were stable in the presence of H 2, which fully reduced the copper oxide at 400–450 K. In CsO x/Cu(111), the CsO x nanoclusters were dispersed all over the metallic copper in no particular order. The CsO x species had an averagemore » width of 2 nm and ~1 Å height. The CsO x/Cu(111) systems exhibited the highest activity for the binding and dissociation of CO 2, indicating that the CsO x-copper interface plays a key role in alcohol synthesis.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [4]; ORCiD logo [1];  [2]; ORCiD logo [5]
  1. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Stony Brook Univ., NY (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  5. tony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE
OSTI Identifier:
1597254
Alternate Identifier(s):
OSTI ID: 1593179
Report Number(s):
BNL-213596-2020-JAAM
Journal ID: ISSN 0021-9606
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 152; Journal Issue: 4; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Cesium; copper oxide; CO2 hydrogenation

Citation Formats

Hamlyn, Rebecca, Mahapatra, Mausumi, Orozco, Ivan, Hunt, Adrian, Waluyo, Iradwikanari, White, Michael G., Senanayake, Sanjaya D., and Rodriguez, José. Morphology and chemical behavior of model CsOx/Cu2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO2 and H2. United States: N. p., 2020. Web. doi:10.1063/1.5129152.
Hamlyn, Rebecca, Mahapatra, Mausumi, Orozco, Ivan, Hunt, Adrian, Waluyo, Iradwikanari, White, Michael G., Senanayake, Sanjaya D., & Rodriguez, José. Morphology and chemical behavior of model CsOx/Cu2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO2 and H2. United States. doi:10.1063/1.5129152.
Hamlyn, Rebecca, Mahapatra, Mausumi, Orozco, Ivan, Hunt, Adrian, Waluyo, Iradwikanari, White, Michael G., Senanayake, Sanjaya D., and Rodriguez, José. Wed . "Morphology and chemical behavior of model CsOx/Cu2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO2 and H2". United States. doi:10.1063/1.5129152.
@article{osti_1597254,
title = {Morphology and chemical behavior of model CsOx/Cu2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO2 and H2},
author = {Hamlyn, Rebecca and Mahapatra, Mausumi and Orozco, Ivan and Hunt, Adrian and Waluyo, Iradwikanari and White, Michael G. and Senanayake, Sanjaya D. and Rodriguez, José},
abstractNote = {Cs is a promoter of Cu-based catalysts for the synthesis of alcohols from CO2 hydrogenation. Scanning tunneling microscopy and ambient-pressure x-ray photoelectron spectroscopy were used to study the morphology and chemical properties of surfaces generated by the deposition of cesium on Cu2O/Cu(111) and Cu(111) substrates. CsOx nanostructures were formed after Cs metal was deposited on Cu2O/Cu(111) at 300 K. The formed CsOx protrude over the surface of copper oxide by 2–4 Å, with the dimension at the base of the nanostructures being in the range of 1–3 nm. Heating to elevated temperature induced significant changes in the size and dispersion of the CsOx nanostructures, and there was a clear reconstruction of the copper oxide substrate, which then exhibited long range order with a hexagonally packed structure. The as-deposited and annealed surfaces of CsOx/Cu2O/Cu(111) were more reactive toward CO2 than plain Cu2O/Cu(111) or clean Cu(111). Yet, none of them were stable in the presence of H2, which fully reduced the copper oxide at 400–450 K. In CsOx/Cu(111), the CsOx nanoclusters were dispersed all over the metallic copper in no particular order. The CsOx species had an average width of 2 nm and ~1 Å height. The CsOx/Cu(111) systems exhibited the highest activity for the binding and dissociation of CO2, indicating that the CsOx-copper interface plays a key role in alcohol synthesis.},
doi = {10.1063/1.5129152},
journal = {Journal of Chemical Physics},
number = 4,
volume = 152,
place = {United States},
year = {2020},
month = {1}
}

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