Manganese Oxide as a Promoter for Copper Catalysts in CO2 and CO Hydrogenation

Remco Dalebout, Laura Barberis, Nienke L. Visser, Jessi E.S. van der Hoeven, Ad M.J. van der Eerden, Joseph A. Stewart, Florian Meirer, Krijn P. de Jong, Petra E. de Jongh*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

In this work, we discuss the role of manganese oxide as a promoter in Cu catalysts supported on graphitic carbon during hydrogenation of CO2 and CO. MnOx is a selectivity modifier in an H2/CO2 feed and is a highly effective activity promoter in an H2/CO feed. Interestingly, the presence of MnOx suppresses the methanol formation from CO2 (TOF of 0.7 ⋅ 10−3 s−1 at 533 K and 40 bar) and enhances the low-temperature reverse water-gas shift reaction (TOF of 5.7 ⋅ 10−3 s−1) with a selectivity to CO of 87 %C. Using time-resolved XAS at high temperatures and pressures, we find significant absorption of CO2 to the MnO, which is reversed if CO2 is removed from the feed. This work reveals fundamental differences in the promoting effect of MnOx and ZnOx and contributes to a better understanding of the role of reducible oxide promoters in Cu-based hydrogenation catalysts.

Original languageEnglish
Article numbere202200451
Number of pages13
JournalChemCatChem
Volume14
Issue number19
DOIs
Publication statusPublished - 10 Oct 2022

Bibliographical note

Funding Information:
We are grateful for the help of Giorgio Totarella and Xavier Carrier during the XAS experiments. We acknowledge SOLEIL for provision of synchrotron radiation facilities, and we would like to thank Camille La Fontaine and Valérie Briois for assistance in using the ROCK beamline (proposal ID 20190640). The work at ROCK was supported by a public grant overseen by the French National Research Agency (ANR) as part of the program (reference: ANR10‐EQPX45). This project has received funding from the European Research Council (ERC), ERC‐2014‐CoG, project number 648991. LB gratefully acknowledge the Consortium on Metal Nanocatalysts funded by TotalEnergies OneTech Belgium, TRTF Contract Ref IPA‐5443. Inventissements d'Avenir

Funding Information:
We are grateful for the help of Giorgio Totarella and Xavier Carrier during the XAS experiments. We acknowledge SOLEIL for provision of synchrotron radiation facilities, and we would like to thank Camille La Fontaine and Valérie Briois for assistance in using the ROCK beamline (proposal ID 20190640). The work at ROCK was supported by a public grant overseen by the French National Research Agency (ANR) as part of the Inventissements d'Avenir program (reference: ANR10-EQPX45). This project has received funding from the European Research Council (ERC), ERC-2014-CoG, project number 648991. LB gratefully acknowledge the Consortium on Metal Nanocatalysts funded by TotalEnergies OneTech Belgium, TRTF Contract Ref IPA-5443.

Publisher Copyright:
© 2022 The Authors. ChemCatChem published by Wiley-VCH GmbH.

Funding

We are grateful for the help of Giorgio Totarella and Xavier Carrier during the XAS experiments. We acknowledge SOLEIL for provision of synchrotron radiation facilities, and we would like to thank Camille La Fontaine and Valérie Briois for assistance in using the ROCK beamline (proposal ID 20190640). The work at ROCK was supported by a public grant overseen by the French National Research Agency (ANR) as part of the program (reference: ANR10‐EQPX45). This project has received funding from the European Research Council (ERC), ERC‐2014‐CoG, project number 648991. LB gratefully acknowledge the Consortium on Metal Nanocatalysts funded by TotalEnergies OneTech Belgium, TRTF Contract Ref IPA‐5443. Inventissements d'Avenir We are grateful for the help of Giorgio Totarella and Xavier Carrier during the XAS experiments. We acknowledge SOLEIL for provision of synchrotron radiation facilities, and we would like to thank Camille La Fontaine and Valérie Briois for assistance in using the ROCK beamline (proposal ID 20190640). The work at ROCK was supported by a public grant overseen by the French National Research Agency (ANR) as part of the Inventissements d'Avenir program (reference: ANR10-EQPX45). This project has received funding from the European Research Council (ERC), ERC-2014-CoG, project number 648991. LB gratefully acknowledge the Consortium on Metal Nanocatalysts funded by TotalEnergies OneTech Belgium, TRTF Contract Ref IPA-5443.

Keywords

  • Catalyst
  • Hydrogenation
  • Operando spectroscopy
  • Promoter
  • X-ray absorption spectroscopy

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