Oxide–Support Interactions

Bergwerff, Jaap A.; Weckhuysen, Bert M.

doi:10.1002/9783527610044.hetcat0062

Cited by 3 publications

(1 citation statement)

References 72 publications

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“…[2][3][4] Unfortunately, most characterization techniques either give a partial picture of the surface structure, or appear to be silent if the creation of metal-oxygen-support bonds does not significantly perturb the first coordination sphere of the metal. 5 As an example, Raman spectroscopy allows one to differentiate between mono-oxo and di-oxo surface species, 6 and polymeric vs. monomeric species. But this technique is much less convincing when the symmetry is concerned (octahedral vs. tetrahedral) and nearly blind with respect to metaloxygen-support bonds, even in the simplest case, i.e.…”

Section: Introductionmentioning

confidence: 99%

EXAFS spectroscopy as a tool to probe metal–support interaction and surface molecular structures in oxide-supported catalysts: application to Al2O3-supported Ni(ii) complexes and ZrO2-supported tungstates

Carrier

Marceau

Carabineiro

et al. 2009

Phys. Chem. Chem. Phys.

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Section: Introductionmentioning

confidence: 99%

EXAFS spectroscopy as a tool to probe metal–support interaction and surface molecular structures in oxide-supported catalysts: application to Al2O3-supported Ni(ii) complexes and ZrO2-supported tungstates

Carrier

Marceau

Carabineiro

et al. 2009

Phys. Chem. Chem. Phys.

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Role of Zirconia in Indium Oxide-Catalyzed CO₂Hydrogenation to Methanol

et al. 2019

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Monoclinic zirconia has been uncovered as a carrier able to substantially boost the activity of indium oxide for CO2 hydrogenation to methanol. Here, electronic, geometric, and interfacial phenomena associated with this unique effect are investigated. Generating mixed In-Zr oxides by coprecipitation does not improve performance, excluding a primary role of electronic parameters.Since even only 1 mol% of indium stabilizes the metastable tetragonal phase of zirconia, the relevance of its crystalline structure is explored in impregnated solids. Both tetragonal and monoclinic ZrO2 permit epitaxial growth of In2O3, but a delicate lattice mismatching leads to a slightly lower dispersion of the oxide on the second, which is observed in the form of subnanometric islands on the carrier. More importantly, compressive and tensile forces are exerted on In2O3, respectively, which inhibit and foster oxygen vacancy formation, in line with the low and greatly enhanced indium-specific activity of the catalysts prepared with the two polymorphs.Hence, a deposition synthesis method is essential to unlock the role of monoclinic zirconia.According to analyses with reference In2O3-based catalysts supported on alumina and ceria, which display diverse ability to activate CO2 on their surface, the direct participation of monoclinic zirconia in a parallel pathway to methanol is put forward as a second origin of activity boosting.The latter is likely enabled by the abundancy of indium active sites vicinal to the interface and/or by a more favorable CO2 adsorption geometry onto this carrier or onto an alternative bimetallic site possibly produced.

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Nanostructure of nickel-promoted indium oxide catalysts drives selectivity in CO2 hydrogenation

et al. 2021

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Metal promotion in heterogeneous catalysis requires nanoscale-precision architectures to attain maximized and durable benefits. Herein, we unravel the complex interplay between nanostructure and product selectivity of nickel-promoted In2O3 in CO2 hydrogenation to methanol through in-depth characterization, theoretical simulations, and kinetic analyses. Up to 10 wt.% nickel, InNi3 patches are formed on the oxide surface, which cannot activate CO2 but boost methanol production supplying neutral hydrogen species. Since protons and hydrides generated on In2O3 drive methanol synthesis rather than the reverse water-gas shift but radicals foster both reactions, nickel-lean catalysts featuring nanometric alloy layers provide a favorable balance between charged and neutral hydrogen species. For nickel contents >10 wt.%, extended InNi3 structures favor CO production and metallic nickel additionally present produces some methane. This study marks a step ahead towards green methanol synthesis and uncovers chemistry aspects of nickel that shall spark inspiration for other catalytic applications.

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Oxide–Support Interactions

Abstract: The sections in this article are Acknowledgments

Cited by 3 publications

References 72 publications

EXAFS spectroscopy as a tool to probe metal–support interaction and surface molecular structures in oxide-supported catalysts: application to Al2O3-supported Ni(ii) complexes and ZrO2-supported tungstates

EXAFS spectroscopy as a tool to probe metal–support interaction and surface molecular structures in oxide-supported catalysts: application to Al2O3-supported Ni(ii) complexes and ZrO2-supported tungstates

Role of Zirconia in Indium Oxide-Catalyzed CO₂Hydrogenation to Methanol

Nanostructure of nickel-promoted indium oxide catalysts drives selectivity in CO2 hydrogenation

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Oxide–Support Interactions

Abstract: The sections in this article are Acknowledgments

Cited by 3 publications

References 72 publications

EXAFS spectroscopy as a tool to probe metal–support interaction and surface molecular structures in oxide-supported catalysts: application to Al2O3-supported Ni(ii) complexes and ZrO2-supported tungstates

EXAFS spectroscopy as a tool to probe metal–support interaction and surface molecular structures in oxide-supported catalysts: application to Al2O3-supported Ni(ii) complexes and ZrO2-supported tungstates

Role of Zirconia in Indium Oxide-Catalyzed CO2Hydrogenation to Methanol

Nanostructure of nickel-promoted indium oxide catalysts drives selectivity in CO2 hydrogenation

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Product

Resources

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Role of Zirconia in Indium Oxide-Catalyzed CO₂Hydrogenation to Methanol