Online citations, reference lists, and bibliographies.

CO2 -to-Methanol Hydrogenation On Zirconia-Supported Copper Nanoparticles: Reaction Intermediates And The Role Of The Metal-Support Interface.

Kim Larmier, Wei-Chih Liao, Shohei Tada, Erwin Lam, René Verel, A. B. Bansode, Atsushi Urakawa, Aleix Comas-Vives, Christophe Copéret
Published 2017 · Medicine, Chemistry
Cite This
Download PDF
Analyze on Scholarcy
Share
Methanol synthesis by CO2 hydrogenation is a key process in a methanol-based economy. This reaction is catalyzed by supported copper nanoparticles and displays strong support or promoter effects. Zirconia is known to enhance both the methanol production rate and the selectivity. Nevertheless, the origin of this observation and the reaction mechanisms associated with the conversion of CO2 to methanol still remain unknown. A mechanistic study of the hydrogenation of CO2 on Cu/ZrO2 is presented. Using kinetics, in situ IR and NMR spectroscopies, and isotopic labeling strategies, surface intermediates evolved during CO2 hydrogenation were observed at different pressures. Combined with DFT calculations, it is shown that a formate species is the reaction intermediate and that the zirconia/copper interface is crucial for the conversion of this intermediate to methanol.
This paper references
10.1021/ACSCATAL.6B01805
Role of the Cu-ZrO2 Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO2 and H2
Insoo Ro (2016)
10.1023/A:1018916806816
Effects of zirconia promotion on the activity of Cu/SiO2 for methanol synthesis from CO/H2 and CO2/H2
Ian Anthony Fisher (1997)
10.1002/anie.201411581
Formation of a ZnO overlayer in industrial Cu/ZnO/Al2 O3 catalysts induced by strong metal-support interactions.
Thomas Lunkenbein (2015)
10.1021/ACSCATAL.6B00822
CO2 Activation on Ni/γ–Al2O3 Catalysts by First-Principles Calculations: From Ideal Surfaces to Supported Nanoparticles
Marius-Christian Silaghi (2016)
10.1021/acscatal.5b02060
Surface-Bound Intermediates in Low-Temperature Methanol Synthesis on Copper: Participants and Spectators
Yong Yang (2015)
10.1039/c4cs00122b
Recycling of carbon dioxide to methanol and derived products - closing the loop.
Alain Goeppert (2014)
10.1002/cctc.201500123
The Mechanism of CO and CO2 Hydrogenation to Methanol over Cu-Based Catalysts
Felix Studt (2015)
10.1126/science.aaf0718
Quantifying the promotion of Cu catalysts by ZnO for methanol synthesis
Sebastian Kuld (2016)
10.1016/0039-6028(89)90266-5
The adsorption of atomic hydrogen on Cu(111) investigated by reflection-absorption infrared spectroscopy, electron energy loss spectroscopy and low energy electron diffraction
Elaine Marie Mccash (1989)
10.1021/jp100864j
Identification of the Active Cu Phase in the Water−Gas Shift Reaction over Cu/ZrO2 from First Principles
Qian-Lin Tang (2010)
10.1126/science.1219831
The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts
Malte Behrens (2012)
10.1016/j.apcata.2008.07.028
Solid-state interactions, adsorption sites and functionality of Cu-ZnO/ZrO2 catalysts in the CO2 hydrogenation to CH3OH
Francesco Arena (2008)
10.1002/anie.201311073
Quantification of zinc atoms in a surface alloy on copper in an industrial-type methanol synthesis catalyst.
Sebastian Kuld (2014)
10.1002/ange.201301419
Die Rolle der Oxidkomponente für die Entwicklung von Kupfer-Komposit-Katalysatoren zur Synthese von Methanol
Stefan Zander (2013)
10.1021/la00099a005
Infrared study of syngas adsorption on zirconia
Eugenio. Guglielminotti (1990)
10.1021/jp209898q
Revealing the Surface Reactivity of Zirconia by Periodic DFT Calculations
Olga A Syzgantseva (2012)
10.1039/c4sc02087a
Hydrogenation of carbon dioxide to methanol using a homogeneous ruthenium–Triphos catalyst: from mechanistic investigations to multiphase catalysis† †Electronic supplementary information (ESI) available: Experimental procedures, analytical data. CCDC 1014053. For ESI and crystallographic data in CIF
Sebastian Wesselbaum (2015)
10.1021/acs.chemrev.5b00373
Surface Organometallic and Coordination Chemistry toward Single-Site Heterogeneous Catalysts: Strategies, Methods, Structures, and Activities.
Christophe Copéret (2016)
10.1039/C2TC00796G
Cu nanoparticles on 2D and 3D silica substrates: controlled size and density, and critical size in catalytic silicon nanowire growth
Arthur Roussey (2013)
10.1021/jacs.6b05791
Optimizing Binding Energies of Key Intermediates for CO2 Hydrogenation to Methanol over Oxide-Supported Copper.
Shyam Kattel (2016)
10.1126/science.1253057
Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2
Jesús Graciani (2014)
10.1021/acscatal.5b01994
Microscopic View of the Active Sites for Selective Dehydrogenation of Formic Acid on Cu(111)
Matthew D. Marcinkowski (2015)
10.1016/J.CEJ.2016.02.069
CO2 hydrogenation to methanol over Cu/ZrO2 catalysts: Effects of zirconia phases
Thongthai Witoon (2016)
10.1016/0926-860X(95)00305-3
Development of copper/zinc oxide-based multicomponent catalysts for methanol synthesis from carbon dioxide and hydrogen
Masahiro Saitȏ (1996)
10.1016/j.apcatb.2015.04.032
Stepwise tuning of metal-oxide and acid sites of CuZnZr-MFI hybrid catalysts for the direct DME synthesis by CO2 hydrogenation
Francesco Frusteri (2015)
10.1063/1.4816515
Adsorption of hydrogen on the surface and sub-surface of Cu(111).
Kumudu K. Mudiyanselage (2013)
10.1023/A:1019071103433
IR study on migration of 18OCH3 species on ZrO2
Feng Ouyang (1998)
10.1021/jp103463s
Hydrogen Adsorption on Monoclinic (1̅11) and (1̅01) ZrO2 Surfaces: A Periodic ab Initio Study
Olga A. Syzgantseva (2010)
10.1002/anie.201301419
The role of the oxide component in the development of copper composite catalysts for methanol synthesis.
Stefan Zander (2013)



This paper is referenced by
10.1016/J.JECHEM.2017.10.011
Rational design of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide
Baohua Zhang (2017)
10.1016/j.cattod.2019.08.049
Conversion of CO2 to C1 chemicals: Catalyst design, kinetics and mechanism aspects of the reactions
Ashok Kumar Jangam (2019)
10.1021/jacs.6b12981
Active Sites in Supported Single-Site Catalysts: An NMR Perspective.
Christophe Copéret (2017)
10.1016/S1872-2067(17)62966-8
ZnO-ZrO 2 solid solution catalyst for highly selective hydrogenation of CO 2 to methanol
Tao Zhang (2017)
10.1016/j.apsusc.2020.146481
Mechanistic insight into the catalytically active phase of CO2 hydrogenation on Cu/ZnO catalyst
Xiao-Kuan Wu (2020)
10.1016/J.CJCHE.2018.07.008
Recent advances on the reduction of CO2 to important C2 + oxygenated chemicals and fuels
Jiachen Li (2018)
10.1016/J.APSUSC.2017.10.097
Theoretical study of the promotional effect of ZrO 2 on In 2 O 3 catalyzed methanol synthesis from CO 2 hydrogenation
Minhua Zhang (2018)
10.1016/j.jcat.2019.10.013
Lewis acidic supports promote the selective hydrogenation of carbon dioxide to methyl formate in the presence of methanol over Ag catalysts
Juan José Corral‐Pérez (2019)
10.1016/J.JCAT.2017.04.021
Ag addition to CuO-ZrO2 catalysts promotes methanol synthesis via CO2 hydrogenation
Shohei Tada (2017)
10.1002/AIC.16717
Influences of particle size and crystallinity of highly loaded CuO/ZrO2 on CO2 hydrogenation to methanol
Kakeru Fujiwara (2019)
10.3929/ETHZ-B-000302511
Research Update: Distribution and stabilization of Pd catalysts in porous carbon-based supports by aggregation of pre-doped colloidal particles
Anna Beltzung (2018)
10.1016/J.NANOEN.2017.08.049
Energy related CO2 conversion and utilization: Advanced materials/nanomaterials, reaction mechanisms and technologies
Yun Zheng (2017)
10.1016/j.jcou.2020.02.009
Power-to-Liquid catalytic CO2 valorization into fuels and chemicals: focus on the Fischer-Tropsch route
Carlotta Panzone (2020)
10.1016/J.APCATB.2018.10.059
Enhanced low-temperature performance of CO2 methanation over mesoporous Ni/Al2O3-ZrO2 catalysts
Jianghui Lin (2019)
10.1016/bs.acat.2019.10.002
Recent advances in catalytic CO2 hydrogenation to alcohols and hydrocarbons
Xiaowa Nie (2019)
10.1016/J.CATTOD.2018.10.038
Structure control on kinetics of copper reduction in Zr–containing mixed oxides during catalytic hydrogenation of carbon oxides to methanol
Giuseppe Bonura (2020)
10.1038/s41560-019-0491-2
Fuels and energy carriers from single-site catalysts prepared via surface organometallic chemistry
Christophe Copéret (2019)
10.1016/J.MCAT.2019.110499
CO2 hydrogenation over acid-activated Attapulgite/Ce0.75Zr0.25O2 nanocomposite supported Cu-ZnO based catalysts
Haijun Guo (2019)
10.1016/J.APCATB.2019.03.003
Photo-assisted methanol synthesis via CO2 reduction under ambient pressure over plasmonic Cu/ZnO catalysts
Zhou-jun Wang (2019)
10.1016/J.CATTOD.2018.02.055
CO2 Hydrogenation to Methanol on Pd-Cu Bimetallic Catalysts: H2/CO2 Ratio Dependence and Surface Species
Xiao Jiang (2018)
10.1016/J.APSUSC.2018.04.128
Theoretical study of methanol synthesis from CO 2 hydrogenation on PdCu 3 (111) surface
Lingna Liu (2018)
10.1039/d0ra00347f
Effective hydrogenation of carbonates to produce methanol over a ternary Cu/Zn/Al catalyst
Jiachen Li (2020)
10.1021/jacs.7b05362
Tuning Selectivity of CO2 Hydrogenation Reactions at the Metal/Oxide Interface.
Shyam Kattel (2017)
10.1021/jacs.8b08505
Decisive Role of Perimeter Sites in Silica-Supported Ag Nanoparticles in Selective Hydrogenation of CO2 to Methyl Formate in the Presence of Methanol.
Juan José Corral-Pérez (2018)
10.1016/J.JCAT.2019.05.023
Modelling the CO2 hydrogenation reaction over Co, Ni and Ru/Al2O3
Robin Mutschler (2019)
10.1002/CCTC.201900517
Construction of Pd/BiOCl Catalyst for Highly‐selective Synthesis of Benzoin Ethyl Ether by Chlorine Promoted Coupling Reaction
Qinglin Yuan (2019)
10.1016/j.cclet.2020.05.031
Comparative study of CO2 hydrogenation to methanol on cubic bixbyite-type and rhombohedral corundum-type indium oxide
Bin Yang (2020)
10.1002/SLCT.201900860
CO2 Hydrogenation to Methanol via In‐situ Reduced Cu/ZnO Catalyst Prepared by Formic acid Assisted Grinding
Peng Xian Lu (2019)
10.3390/ma12233902
Methanol Synthesis from CO2: A Review of the Latest Developments in Heterogeneous Catalysis
Rut Guil-López (2019)
10.1039/c8dt00186c
Clean chlorination of silica surfaces by a single-site substitution approach.
N. P. Maity (2018)
10.1002/cssc.201902485
Capsule-structured copper-zinc catalyst for highly efficient hydrogenation of carbon dioxide to methanol.
Yongle Guo (2019)
10.1039/c9cy02287b
A systematic theoretical study of the water gas shift reaction on the Pt/ZrO2 interface and Pt(111) face: key role of a potassium additive
Yan-Xin Wang (2020)
See more
Semantic Scholar Logo Some data provided by SemanticScholar