A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in ‘Metal Efficient’ Palladium/In2O3/Al2O3 Catalysts for CO2 Hydrogenation

Author:

Potter Matthew E.12,Mediavilla Madrigal Sofia23,Campbell Emma23,Allen Lisa J.12,Vyas Urvashi12,Parry Stephen4,García‐Zaragova Adrián5,Martínez‐Prieto Luis M.56,Oña‐Burgos Pascual5,Lützen Mads7,Damsgaard Christian D.78,Rodríguez‐Castellón Enrique9,Schiaroli Nicola10,Fornasari Giuseppe1011,Benito Patricia1011,Beale Andrew M.12ORCID

Affiliation:

1. Chemistry Department University College London 20 Gordon Street London WC1H 0AJ UK

2. UK Catalysis Hub Research Complex at Harwell Rutherford Appleton Laboratory Didcot OX11 0FA UK

3. Cardiff Catalysis Institute School of Chemistry Cardiff University Cardiff CF10 3AT UK

4. Diamond Light Source Rutherford Appleton Laboratory Didcot OX11 0FA UK

5. ITQ, Instituto de Tecnología Química Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) Av. de los Naranjos S/N 46022 Valencia Spain

6. IIQ, Instituto de Investigaciones Químicas CSIC-Universidad de Sevilla Departamento de Química Inorgánica; Avda Americo Vespucio 49 41092 Seville Spain

7. National Centre for Nanofabrication and Charaterisation Technical University of Denmark Fysikvej Building 307 2800 Kgs. Lyngby Denmark

8. Department of Physics Technical University of Denmark Fysikvej Building 311 2800 Kgs. Lyngby Denmark

9. Departamento de Química Inorgánica Universidad de Málaga Facultad de Ciencias. 29071 Málaga Spain

10. Dipartimento di Chimica Industriale “Toso Montanari” Università di Bologna Alma Mater Studiorum Viale Risorgimento 4 40136 Bologna Italy

11. Center for Chemical Catalysis—C3 Università di Bologna Alma Mater Studiorum Viale Risorgimento 4 40136 Bologna Italy

Abstract

AbstractCO2 hydrogenation to methanol has the potential to serve as a sustainable route to a wide variety of hydrocarbons, fuels and plastics in the quest for net zero. Synergistic Pd/In2O3 (Palldium on Indium Oxide) catalysts show high CO2 conversion and methanol selectivity, enhancing methanol yield. The identity of the optimal active site for this reaction is unclear, either as a Pd−In alloy, proximate metals, or distinct sites. In this work, we demonstrate that metal‐efficient Pd/In2O3 species dispersed on Al2O3 can match the performance of pure Pd/In2O3 systems. Further, we follow the evolution of both Pd and In sites, and surface species, under operando reaction conditions using X‐ray Absorption Spectroscpy (XAS) and infrared (IR) spectroscopy. In doing so, we can determine both the nature of the active sites and the influence on the catalytic mechanism.

Funder

Engineering and Physical Sciences Research Council

H2020 European Research Council

Villum Fonden

Ministerio de Ciencia e Innovación

Diamond Light Source

Publisher

Wiley

Subject

General Chemistry,Catalysis

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