Rationally designed laterally-condensed-catalysts deliver robust activity and selectivity for ethylene production in acetylene hydrogenation
Future carbon management strategies require storage in elemental form, achievable through a sequence of CO<sub>2</sub> 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 SiO<sub>2</sub> 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 kmol<sub>C2H4</sub>/g<sub>Pd</sub>/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.
Authors
- Christoph Scheurer (ORCID: https://orcid.org/0000-0002-7227-8672)
- Shan Jiang (ORCID: https://orcid.org/0000-0003-2419-2011)
- Maurício J. Prieto (ORCID: https://orcid.org/0000-0002-5087-4545)
- Annette Trunschke (ORCID: https://orcid.org/0000-0003-2869-0181)
- Raul Garcia‐Diez (ORCID: https://orcid.org/0009-0000-9374-1083)
- Patrick Zeller
- Afshan Jamshaid (ORCID: https://orcid.org/0000-0001-5983-1544)
- Alexandra M. Dudzinski (ORCID: https://orcid.org/0000-0003-4688-4369)
- Karsten Reuter (ORCID: https://orcid.org/0000-0001-8473-8659)
- Tobias Köhler (ORCID: https://orcid.org/0000-0001-7890-3144)
- Thomas Lunkenbein (ORCID: https://orcid.org/0000-0002-8957-4216)
- Christian Künkel (ORCID: https://orcid.org/0000-0002-0612-1706)
- Sabine Wrabetz
- Maria Dimitrakopoulou (ORCID: https://orcid.org/0000-0002-1349-384X)
- Rutger Schlatmann (ORCID: https://orcid.org/0000-0002-5951-9435)
- Katarzyna Skorupska (ORCID: https://orcid.org/0000-0002-1970-0395)
- Johannes Frisch (ORCID: https://orcid.org/0000-0002-7895-7529)
- H. Kuhlenbeck (ORCID: https://orcid.org/0000-0001-6384-8883)
- Miriam Götte (ORCID: https://orcid.org/0000-0003-0841-8738)
- Olga Vinogradova (ORCID: https://orcid.org/0000-0001-5862-3639)
- Alexander Steigert (ORCID: https://orcid.org/0009-0006-0941-7744)
- Raoul Blume (ORCID: https://orcid.org/0009-0006-4362-339X)
- Daniel Amkreutz (ORCID: https://orcid.org/0000-0002-4589-6598)
- Matuš Stredansky (ORCID: https://orcid.org/0000-0002-4907-1892)
- Daniel Delgado (ORCID: https://orcid.org/0000-0002-2976-3322)
- Franz Schmidt (ORCID: https://orcid.org/0000-0003-0125-2704)
- Wiebke Frandsen
- Beatriz Roldán Cuenya (ORCID: https://orcid.org/0000-0002-8025-307X)
- Pierre Kube (ORCID: https://orcid.org/0000-0001-8311-5919)
- Christian Rohner (ORCID: https://orcid.org/0000-0003-2163-6713)
- Vanessa J. Bukas (ORCID: https://orcid.org/0000-0002-0105-863X)
- Frank Girgsdies (ORCID: https://orcid.org/0000-0002-0994-0686)
- Tathiana Midori Kokumai (ORCID: https://orcid.org/0000-0002-3478-2771)
- Jutta Kröhnert
- F. Eylul Sarac Oztuna (ORCID: https://orcid.org/0000-0003-1195-3774)
- Thomas Schmidt (ORCID: https://orcid.org/0000-0003-4389-2080)
- Adnan Hammud (ORCID: https://orcid.org/0000-0001-5580-7985)
- Marcus Bär (ORCID: https://orcid.org/0000-0001-8581-0691)
- M. Muske
- Manuela Arztmann (ORCID: https://orcid.org/0009-0008-7005-3382)
- Zehua Li (ORCID: https://orcid.org/0000-0003-2518-9287)
- Anna Efimenko (ORCID: https://orcid.org/0000-0003-3906-6747)
- Axel Knop‐Gericke (ORCID: https://orcid.org/0009-0008-1149-4102)
- R. Schlögl
Institutions
- Friedrich-Alexander-Universität Erlangen-Nürnberg (DE)
- Helmholtz-Zentrum Berlin für Materialien und Energie (DE)
- Fritz Haber Institute of the Max Planck Society (DE)
- Helmholtz Institute Erlangen-Nürnberg (DE)
- Max Planck Institute for Chemical Energy Conversion (DE)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-12-10
- DOI
- https://doi.org/10.1038/s41467-024-54784-z
- Citations
- 12
- Primary Topic
- Metal-Organic Frameworks: Synthesis and Applications
- Type
- article
- Field-Weighted Citation Impact
- 1.90
Funders
- Bundesministerium für Bildung und Forschung
- Max-Planck-Gesellschaft
- Helmholtz-Zentrum Berlin für Materialien und Energie