Rationally designed laterally-condensed-catalysts deliver robust activity and selectivity for ethylene production in acetylene hydrogenation
Zehua Li,
Eylül Öztuna,
Katarzyna Skorupska (),
Olga V. Vinogradova,
Afshan Jamshaid,
Alexander Steigert,
Christian Rohner,
Maria Dimitrakopoulou,
Mauricio J. Prieto,
Christian Kunkel,
Matus Stredansky,
Pierre Kube,
Michael Götte,
Alexandra M. Dudzinski,
Frank Girgsdies,
Sabine Wrabetz,
Wiebke Frandsen,
Raoul Blume,
Patrick Zeller,
Martin Muske,
Daniel Delgado,
Shan Jiang,
Franz-Philipp Schmidt,
Tobias Köhler,
Manuela Arztmann,
Anna Efimenko,
Johannes Frisch,
Tathiana M. Kokumai,
Raul Garcia-Diez,
Marcus Bär,
Adnan Hammud,
Jutta Kröhnert,
Annette Trunschke,
Christoph Scheurer,
Thomas Schmidt,
Thomas Lunkenbein,
Daniel Amkreutz,
Helmut Kuhlenbeck,
Vanessa J. Bukas,
Axel Knop-Gericke,
Rutger Schlatmann,
Karsten Reuter,
Beatriz Roldan Cuenya and
Robert Schlögl ()
Additional contact information
Zehua Li: Fritz-Haber Institute of the Max Planck Society
Eylül Öztuna: Fritz-Haber Institute of the Max Planck Society
Katarzyna Skorupska: Fritz-Haber Institute of the Max Planck Society
Olga V. Vinogradova: Fritz-Haber Institute of the Max Planck Society
Afshan Jamshaid: Fritz-Haber Institute of the Max Planck Society
Alexander Steigert: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Christian Rohner: Fritz-Haber Institute of the Max Planck Society
Maria Dimitrakopoulou: Fritz-Haber Institute of the Max Planck Society
Mauricio J. Prieto: Fritz-Haber Institute of the Max Planck Society
Christian Kunkel: Fritz-Haber Institute of the Max Planck Society
Matus Stredansky: Fritz-Haber Institute of the Max Planck Society
Pierre Kube: Fritz-Haber Institute of the Max Planck Society
Michael Götte: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Alexandra M. Dudzinski: Fritz-Haber Institute of the Max Planck Society
Frank Girgsdies: Fritz-Haber Institute of the Max Planck Society
Sabine Wrabetz: Fritz-Haber Institute of the Max Planck Society
Wiebke Frandsen: Fritz-Haber Institute of the Max Planck Society
Raoul Blume: Fritz-Haber Institute of the Max Planck Society
Patrick Zeller: Fritz-Haber Institute of the Max Planck Society
Martin Muske: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Daniel Delgado: Fritz-Haber Institute of the Max Planck Society
Shan Jiang: Fritz-Haber Institute of the Max Planck Society
Franz-Philipp Schmidt: Fritz-Haber Institute of the Max Planck Society
Tobias Köhler: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Manuela Arztmann: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Anna Efimenko: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Johannes Frisch: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Tathiana M. Kokumai: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Raul Garcia-Diez: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Marcus Bär: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Adnan Hammud: Fritz-Haber Institute of the Max Planck Society
Jutta Kröhnert: Fritz-Haber Institute of the Max Planck Society
Annette Trunschke: Fritz-Haber Institute of the Max Planck Society
Christoph Scheurer: Fritz-Haber Institute of the Max Planck Society
Thomas Schmidt: Fritz-Haber Institute of the Max Planck Society
Thomas Lunkenbein: Fritz-Haber Institute of the Max Planck Society
Daniel Amkreutz: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Helmut Kuhlenbeck: Fritz-Haber Institute of the Max Planck Society
Vanessa J. Bukas: Fritz-Haber Institute of the Max Planck Society
Axel Knop-Gericke: Fritz-Haber Institute of the Max Planck Society
Rutger Schlatmann: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Karsten Reuter: Fritz-Haber Institute of the Max Planck Society
Beatriz Roldan Cuenya: Fritz-Haber Institute of the Max Planck Society
Robert Schlögl: Fritz-Haber Institute of the Max Planck Society
Nature Communications, 2024, vol. 15, issue 1, 1-13
Abstract:
Abstract Future carbon management strategies require storage in elemental form, achievable through a sequence of CO2 hydrogenation reactions. Hydrogen is recycled from molecular intermediates by dehydrogenation, and side product acetylene selectively hydrogenated to ethylene. Existing Pd alloy catalysts for gas purification underperform in concentrated feeds, necessitating novel concepts. Atomistic simulations unveil superior selectivity of Pd:C solid solutions that optimize chemisorption energies and preclude sub-surface hydrides, verified here with model thin films. Multiple design criteria deduced from conventional catalysts facilitate synthesizing a self-repairing Pd:C system of a laterally condensed catalyst (LCC). A Pd layer prepared on a designated SiO2 buffer layer enables control of reactive interface, sub-surface volume and extended functional interface towards the buffer. Function and metric are supervised by operando micro-spectroscopy. This catalyst design shows, ethylene productivity >1 kmolC2H4/gPd/hour is reproducibly achieved and benchmarked against known catalysts. Photovoltaics deposition technologies enable scalability on real-world substrates saving active metal. A design-of-experiment approach demonstrates the improvement potential of the LCC approach.
Date: 2024
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54784-z
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DOI: 10.1038/s41467-024-54784-z
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