Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts

Kandemir, Timur; Friedrich, Matthias; Parker, Stewart F.; Studt, Felix; Lennon, David; Schlögl, Robert; Behrens, Malte

doi:10.1039/C6CP00967K

Title: Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts

Abstract

We have investigated methanol synthesis with model supported copper catalysts, Cu/ZnO and Cu/MgO, using CO/H₂ and CO₂/H₂ as feedstocks. Under CO/H₂ both catalysts show chemisorbed methoxy as a stable intermediate, the Cu/MgO catalyst also shows hydroxyls on the support. Under CO₂/H₂ the catalysts behave differently, in that formate is also seen on the catalyst. For the Cu/ZnO catalyst hydroxyls are present on the metal whereas for the Cu/MgO hydroxyls are found on the support. Furthermore, these results are consistent with a recently published model for methanol synthesis and highlight the key role of ZnO in the process.

Authors:

Kandemir, Timur ^[1]; Friedrich, Matthias ^[1]; Parker, Stewart F. ^[2]; Studt, Felix ^[3]; Lennon, David ^[4]; Schlögl, Robert ^[1]; Behrens, Malte ^[5]

Fritz-Haber-Institut der Max Planck-Gesellschaft, Berlin (Germany)
STFC Rutherford Appleton Lab., Didcot (United Kingdom)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of Glasgow, Glasgow (United Kingdom)
Univ. of Duisburg-Essen, Essen (Germany)

Publication Date:: Thu Apr 14 00:00:00 EDT 2016

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1312796

Grant/Contract Number:: NMI3-II Grant number 283883, CP-CSA_INFRA-2008-1.1; AC02-76SF00515

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Physical Chemistry Chemical Physics. PCCP

Additional Journal Information:: Journal Volume: 18; Journal Issue: 26; Journal ID: ISSN 1463-9076

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Kandemir, Timur, Friedrich, Matthias, Parker, Stewart F., Studt, Felix, Lennon, David, Schlögl, Robert, and Behrens, Malte. Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts.  United States: N. p., 2016. 
        Web.  doi:10.1039/C6CP00967K.

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                    Kandemir, Timur, Friedrich, Matthias, Parker, Stewart F., Studt, Felix, Lennon, David, Schlögl, Robert, & Behrens, Malte. Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts.  United States.  https://doi.org/10.1039/C6CP00967K

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                    Kandemir, Timur, Friedrich, Matthias, Parker, Stewart F., Studt, Felix, Lennon, David, Schlögl, Robert, and Behrens, Malte. 2016.  
        "Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts".  United States.  https://doi.org/10.1039/C6CP00967K.  https://www.osti.gov/servlets/purl/1312796.

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@article{osti_1312796,

  title        = {Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts},

  author       = {Kandemir, Timur and Friedrich, Matthias and Parker, Stewart F. and Studt, Felix and Lennon, David and Schlögl, Robert and Behrens, Malte},

  abstractNote = {We have investigated methanol synthesis with model supported copper catalysts, Cu/ZnO and Cu/MgO, using CO/H2 and CO2/H2 as feedstocks. Under CO/H2 both catalysts show chemisorbed methoxy as a stable intermediate, the Cu/MgO catalyst also shows hydroxyls on the support. Under CO2/H2 the catalysts behave differently, in that formate is also seen on the catalyst. For the Cu/ZnO catalyst hydroxyls are present on the metal whereas for the Cu/MgO hydroxyls are found on the support. Furthermore, these results are consistent with a recently published model for methanol synthesis and highlight the key role of ZnO in the process.},

  doi          = {10.1039/C6CP00967K},

  url          = {https://www.osti.gov/biblio/1312796},
  journal      = {Physical Chemistry Chemical Physics. PCCP},

  issn         = {1463-9076},

  number       = 26,

  volume       = 18,

  place        = {United States},

  year         = {Thu Apr 14 00:00:00 EDT 2016},

  month        = {Thu Apr 14 00:00:00 EDT 2016}

}

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Title: Different routes to methanol: Inelastic neutron scattering spectroscopy of adsorbates on supported copper catalysts

Abstract

Citation Formats

Oxide-supported copper catalysts prepared from copper formate: Differences in behavior in methanol synthesis from CO/H2 and CO2/H2 mixtures journal, December 1986

The Role of the Oxide Component in the Development of Copper Composite Catalysts for Methanol Synthesis journal, May 2013

The role of ZnO in Cu/ZnO methanol synthesis catalysts — morphology effect or active site model? journal, February 2001

The role of copper and zinc oxide in methanol synthesis catalysts journal, January 1990

Mechanism of Methanol Synthesis on Cu through CO 2 and CO Hydrogenation journal, February 2011

The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts journal, April 2012

Methanol synthesis by CO and CO2 hydrogenation on Cu/γ-Al2O3 surface in liquid paraffin solution journal, January 2014

Methanol Synthesis journal, January 1980

Mechanism of methanol synthesis from CO2/CO/H2 mixtures over copper/zinc oxide/alumina catalysts: use of14C-labelled reactants journal, April 1987

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An equilibrium model for biomass gasification processes journal, January 1999

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The mechanism of methanol synthesis on copper/zinc oxide/alumina catalysts journal, February 1988

The influence of strongly reducing conditions on strong metal–support interactions in Cu/ZnO catalysts used for methanol synthesis journal, January 2006

Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al 2 O 3 Catalysts Induced by Strong Metal-Support Interactions journal, February 2015

In Situ Study of Catalytic Processes: Neutron Diffraction of a Methanol Synthesis Catalyst at Industrially Relevant Pressure journal, April 2013

Formate synthesis on Cu(100) journal, January 1992

Synthesis and hydrogenation of formate on Cu(100) at high pressures journal, July 1992

Spectroscopic studies of hydrogen adsorbed on zinc oxide (kadox 25) journal, January 1984

Detection of hydrogen-copper clustering in Zn1−x CuxO compounds using neutron scattering methods journal, July 2006

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Vibrational Spectroscopy with Neutrons: A Review of New Directions journal, December 2011

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The adsorption and reaction of methanol on oxidized copper(111) studied by Fourier transform reflection-absorption infrared spectroscopy journal, January 1987

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Methanol Synthesis from CO/CO2/H2over Cu/ZnO/Al2O3at Differential and Finite Conversions journal, March 1998

Oxide-supported copper catalysts prepared from copper formate: Differences in behavior in methanol synthesis from CO/H2 and CO2/H2 mixtures
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The Role of the Oxide Component in the Development of Copper Composite Catalysts for Methanol Synthesis
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The role of copper and zinc oxide in methanol synthesis catalysts
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Mechanism of Methanol Synthesis on Cu through CO ₂ and CO Hydrogenation
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Methanol synthesis by CO and CO2 hydrogenation on Cu/γ-Al2O3 surface in liquid paraffin solution
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Mechanism of methanol synthesis from CO2/CO/H2 mixtures over copper/zinc oxide/alumina catalysts: use of14C-labelled reactants
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Reactions CO, H2 - synthese du methanol sur chromite de zinc etude d'especes chimisorbees a la surface du catalyseur schemas reactionnels possibles
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The influence of strongly reducing conditions on strong metal–support interactions in Cu/ZnO catalysts used for methanol synthesis
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Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al ₂ O ₃ Catalysts Induced by Strong Metal-Support Interactions
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FTIR studies of dynamic surface structural changes in Cu-based methanol synthesis catalysts
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