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

Matthew E. Potter; Sofia Mediavilla Madrigal; Emma Campbell; Lisa J. Allen; Urvashi Vyas; Stephen Parry; Adrián García-Zaragova; Luis M. Martínez-Prieto; Pascual Oña-Burgos; Mads Lützen; Christian D. Damsgaard; Enrique Rodríguez-Castellón; Nicola Schiaroli; Giuseppe Fornasari; Patricia Benito; Andrew M. Beale

doi:10.1002/anie.202312645

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

Matthew E. Potter^*, Sofia Mediavilla Madrigal, Emma Campbell, Lisa J. Allen, Urvashi Vyas, Stephen Parry, Adrián García-Zaragova, Luis M. Martínez-Prieto, Pascual Oña-Burgos, Mads Lützen, Christian D. Damsgaard, Enrique Rodríguez-Castellón, Nicola Schiaroli, Giuseppe Fornasari, Patricia Benito^*, Andrew M. Beale^*

^*Corresponding author for this work

Research output: Contribution to journal › Letter › peer-review

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Abstract

CO₂ 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.

Original language	English
Article number	e202312645
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	45
Number of pages	6
ISSN	1433-7851
DOIs	https://doi.org/10.1002/anie.202312645
Publication status	Published - 2023

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Potter, M. E., Mediavilla Madrigal, S., Campbell, E., Allen, L. J., Vyas, U., Parry, S., García-Zaragova, A., Martínez-Prieto, L. M., Oña-Burgos, P., Lützen, M., Damsgaard, C. D., Rodríguez-Castellón, E., Schiaroli, N., Fornasari, G., Benito, P., & Beale, A. M. (2023). A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in ‘Metal Efficient’ Palladium/In₂O₃/Al₂O₃ Catalysts for CO₂ Hydrogenation. Angewandte Chemie - International Edition, 62(45), Article e202312645. https://doi.org/10.1002/anie.202312645

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title = "A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in {\textquoteleft}Metal Efficient{\textquoteright} Palladium/In2O3/Al2O3 Catalysts for CO2 Hydrogenation",

abstract = "CO2 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.",

author = "Potter, \{Matthew E.\} and \{Mediavilla Madrigal\}, Sofia and Emma Campbell and Allen, \{Lisa J.\} and Urvashi Vyas and Stephen Parry and Adri{\'a}n Garc{\'i}a-Zaragova and Mart{\'i}nez-Prieto, \{Luis M.\} and Pascual O{\~n}a-Burgos and Mads L{\"u}tzen and Damsgaard, \{Christian D.\} and Enrique Rodr{\'i}guez-Castell{\'o}n and Nicola Schiaroli and Giuseppe Fornasari and Patricia Benito and Beale, \{Andrew M.\}",

note = "Publisher Copyright: {\textcopyright} 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

year = "2023",

doi = "10.1002/anie.202312645",

language = "English",

volume = "62",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "John Wiley and Sons Ltd",

number = "45",

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Potter, ME, Mediavilla Madrigal, S, Campbell, E, Allen, LJ, Vyas, U, Parry, S, García-Zaragova, A, Martínez-Prieto, LM, Oña-Burgos, P, Lützen, M, Damsgaard, CD, Rodríguez-Castellón, E, Schiaroli, N, Fornasari, G, Benito, P & Beale, AM 2023, 'A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in ‘Metal Efficient’ Palladium/In₂O₃/Al₂O₃ Catalysts for CO₂ Hydrogenation', Angewandte Chemie - International Edition, vol. 62, no. 45, e202312645. https://doi.org/10.1002/anie.202312645

A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in ‘Metal Efficient’ Palladium/In₂O₃/Al₂O₃ Catalysts for CO₂ Hydrogenation. / Potter, Matthew E.; Mediavilla Madrigal, Sofia; Campbell, Emma et al.
In: Angewandte Chemie - International Edition, Vol. 62, No. 45, e202312645, 2023.

Research output: Contribution to journal › Letter › peer-review

TY - JOUR

T1 - A High Pressure Operando Spectroscopy Examination of Bimetal Interactions in ‘Metal Efficient’ Palladium/In2O3/Al2O3 Catalysts for CO2 Hydrogenation

AU - Potter, Matthew E.

AU - Mediavilla Madrigal, Sofia

AU - Campbell, Emma

AU - Allen, Lisa J.

AU - Vyas, Urvashi

AU - Parry, Stephen

AU - García-Zaragova, Adrián

AU - Martínez-Prieto, Luis M.

AU - Oña-Burgos, Pascual

AU - Lützen, Mads

AU - Damsgaard, Christian D.

AU - Rodríguez-Castellón, Enrique

AU - Schiaroli, Nicola

AU - Fornasari, Giuseppe

AU - Benito, Patricia

AU - Beale, Andrew M.

PY - 2023

Y1 - 2023

N2 - CO2 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.

AB - CO2 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.

U2 - 10.1002/anie.202312645

DO - 10.1002/anie.202312645

M3 - Letter

C2 - 37723118

AN - SCOPUS:85172658854

SN - 1433-7851

VL - 62

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 45

M1 - e202312645

ER -