Morphology and chemical behavior of model CsOx/Cu2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO2 and H2

Hamlyn, Rebecca; Mahapatra, Mausumi; Orozco, Ivan; Hunt, Adrian; Waluyo, Iradwikanari; White, Michael G.; Senanayake, Sanjaya D.; Rodriguez, José

doi:10.1063/1.5129152

Title: Morphology and chemical behavior of model CsO_x/Cu₂O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO₂ and H₂

Abstract

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. CsO_x nanostructures were formed after Cs metal was deposited on Cu₂O/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/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 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 average width of 2 nm and ~1 Å height. The CsO_x/Cu(111) systems exhibited the highestmore »« less

Authors:

^[1]; Mahapatra, Mausumi ^[2]; Orozco, Ivan ^[3]; Hunt, Adrian ^[4];

^[4];

^[1]; Senanayake, Sanjaya D. ^[2];

^[5]

Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
tony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Wed Jan 22 00:00:00 EST 2020

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

OSTI Identifier:: 1597254

Alternate Identifier(s):: OSTI ID: 1593179

Report Number(s):: BNL-213596-2020-JAAM
Journal ID: ISSN 0021-9606; TRN: US2103735

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.

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                    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.  https://doi.org/10.1063/1.5129152

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                    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.  https://doi.org/10.1063/1.5129152.  https://www.osti.gov/servlets/purl/1597254.

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@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         = {Wed Jan 22 00:00:00 EST 2020},

  month        = {Wed Jan 22 00:00:00 EST 2020}

}

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Title: Morphology and chemical behavior of model CsOx/Cu2O/Cu(111) nanocatalysts for methanol synthesis: Reaction with CO2 and H2

Abstract

Citation Formats

Higher Alcohol Synthesis over Double Bed Cs−Cu/ZnO/Cr 2 O 3 Catalysts: Optimizing the Yields of 2-Methyl-1-propanol (Isobutanol) journal, December 1998

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Identification of 5–7 Defects in a Copper Oxide Surface
journal, August 2011

Adsorption of CO 2 on Model Surfaces of Cesium Oxides Determined from First Principles
journal, October 2004

CO 2 insertion into epoxides using cesium salts as catalysts at ambient pressure
journal, January 2019

Higher alcohol and oxygenate synthesis over Cs/Cu/ZnO/M2O3 (M $z.dbnd; Al, Cr) catalysts
journal, March 1989

The effect of preadsorbed K on the size distribution of Au nanoparticles on TiO2(110) surface
journal, August 2006

Low-coverage condensation of K on TiO2(110) 1×1
journal, June 2005

Production of Methanol and Isobutyl Alcohol Mixtures over Double-Bed Cesium-Promoted Cu/ZnO/Cr 2 O 3 and ZnO/Cr 2 O 3 Catalysts
journal, January 1996

Hydrogenation of CO ₂ on ZnO/Cu(100) and ZnO/Cu(111) Catalysts: Role of Copper Structure and Metal–Oxide Interface in Methanol Synthesis
journal, August 2017

Cesium removal from contaminated sand by supercritical CO 2 extraction
journal, March 2016

Autocatalytic Reduction of a Cu ₂ O/Cu(111) Surface by CO: STM, XPS, and DFT Studies
journal, July 2010

Adsorption of carbon monoxide carbon dioxide on clean and cesium-covered copper(110)
journal, June 1989

Hydrogen Chemisorption on Potassium Promoted Supported Ruthenium Catalysts
journal, April 1994

Oxidation of cesium multilayers
journal, October 1993

Kinetics and mechanism of the water-gas shift reaction catalysed by the clean and Cs-promoted Cu(110) surface: a comparison with Cu(111)
journal, January 1990

Oxidation of Cu(111): two new oxygen induced reconstructions
journal, December 1991

A model study of alkali promotion of water-gas shift catalysts: Cs/Cu(111)
journal, August 1987

The Mechanism of Potassium Promoter: Enhancing the Stability of Active Surfaces
journal, June 2011

A model study of alkali promotion of water-gas shift catalysts: Cs/Cu(111)
journal, August 1987