Rationally designed laterally-condensed-catalysts deliver robust activity and selectivity for ethylene production in acetylene hydrogenation

Autor: 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, Robert Schlögl
Jazyk: angličtina
Rok vydání: 2024
Předmět:
Zdroj: Nature Communications, Vol 15, Iss 1, Pp 1-13 (2024)
Druh dokumentu: article
ISSN: 2041-1723
DOI: 10.1038/s41467-024-54784-z
Popis: 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.
Databáze: Directory of Open Access Journals
Externí odkaz: