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

Matthias S. Frei, Cecilia Mondelli, Rodrigo García-Muelas, Jordi Morales-Vidal, Michelle Philipp, Olga V. Safonova, Núria López, Joseph A. Stewart, Daniel Curulla Ferré and Javier Pérez-Ramírez ()
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Matthias S. Frei: Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich
Cecilia Mondelli: Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich
Rodrigo García-Muelas: The Barcelona Institute of Science and Technology
Jordi Morales-Vidal: The Barcelona Institute of Science and Technology
Michelle Philipp: Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich
Olga V. Safonova: Paul Scherrer Institute
Núria López: The Barcelona Institute of Science and Technology
Joseph A. Stewart: Total Research & Technology Feluy, Zone Industrielle Feluy C
Daniel Curulla Ferré: Total Research & Technology Feluy, Zone Industrielle Feluy C
Javier Pérez-Ramírez: Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-22224-x

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