Flame-made ternary Pd-In2O3-ZrO2 catalyst with enhanced oxygen vacancy generation for CO2 hydrogenation to methanol

Thaylan Pinheiro Araújo, Cecilia Mondelli, Mikhail Agrachev, Tangsheng Zou, Patrik O. Willi, Konstantin M. Engel, Robert N. Grass, Wendelin J. Stark, Olga V. Safonova, Gunnar Jeschke, Sharon Mitchell and Javier Pérez-Ramírez ()
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Thaylan Pinheiro Araújo: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Cecilia Mondelli: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Mikhail Agrachev: Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zurich
Tangsheng Zou: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Patrik O. Willi: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Konstantin M. Engel: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Robert N. Grass: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Wendelin J. Stark: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Olga V. Safonova: Paul Scherrer Institute
Gunnar Jeschke: Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zurich
Sharon Mitchell: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich
Javier Pérez-Ramírez: Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Palladium promotion and deposition on monoclinic zirconia are effective strategies to boost the performance of bulk In2O3 in CO2-to-methanol and could unlock superior reactivity if well integrated into a single catalytic system. However, harnessing synergic effects of the individual components is crucial and very challenging as it requires precise control over their assembly. Herein, we present ternary Pd-In2O3-ZrO2 catalysts prepared by flame spray pyrolysis (FSP) with remarkable methanol productivity and improved metal utilization, surpassing their binary counterparts. Unlike established impregnation and co-precipitation methods, FSP produces materials combining low-nuclearity palladium species associated with In2O3 monolayers highly dispersed on the ZrO2 carrier, whose surface partially transforms from a tetragonal into a monoclinic-like structure upon reaction. A pioneering protocol developed to quantify oxygen vacancies using in situ electron paramagnetic resonance spectroscopy reveals their enhanced generation because of this unique catalyst architecture, thereby rationalizing its high and sustained methanol productivity.

Date: 2022
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DOI: 10.1038/s41467-022-33391-w

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