Reaction-Induced Metal-Metal Oxide Interactions in Pd-In 2 O 3 /ZrO 2 Catalysts Drive Selective and Stable CO 2 Hydrogenation to Methanol.

Autor: Araújo TP; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland., Morales-Vidal J; Institute of Chemical Research of Catalonia (ICIQ-CERCA), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.; Universitat Rovira i Virgili, Av. Catalunya 35, 43002, Tarragona, Spain., Giannakakis G; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland., Mondelli C; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland., Eliasson H; Electron Microscopy Center, Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600, Dübendorf, Switzerland., Erni R; Electron Microscopy Center, Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600, Dübendorf, Switzerland., Stewart JA; TotalEnergies OneTech Belgium, Zone Industrielle Feluy C, 7181, Seneffe, Belgium., Mitchell S; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland., López N; Institute of Chemical Research of Catalonia (ICIQ-CERCA), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain., Pérez-Ramírez J; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2023 Oct 16; Vol. 62 (42), pp. e202306563. Date of Electronic Publication: 2023 Jul 27.
DOI: 10.1002/anie.202306563
Abstrakt: Ternary Pd-In 2 O 3 /ZrO 2 catalysts exhibit technological potential for CO 2 -based methanol synthesis, but developing scalable systems and comprehending complex dynamic behaviors of the active phase, promoter, and carrier are key for achieving high productivity. Here, we show that the structure of Pd-In 2 O 3 /ZrO 2 systems prepared by wet impregnation evolves under CO 2 hydrogenation conditions into a selective and stable architecture, independent of the order of addition of Pd and In phases on the zirconia carrier. Detailed operando characterization and simulations reveal a rapid restructuring driven by the metal-metal oxide interaction energetics. The proximity of InPd x alloy particles decorated by InO x layers in the resulting architecture prevents performance losses associated with Pd sintering. The findings highlight the crucial role of reaction-induced restructuring in complex CO 2 hydrogenation catalysts and offer insights into the optimal integration of acid-base and redox functions for practical implementation.
(© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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