Nanostructuring unlocks high performance of platinum single-atom catalysts for stable vinyl chloride production.
- Kaiser SK Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland.
- Fako E Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007 Tarragona, Spain.
- Manzocchi G Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland.
- Krumeich F Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland.
- Hauert R Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland.
- Clark AH Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
- Safonova OV Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
- López N Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007 Tarragona, Spain.
- Pérez-Ramírez J Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland.
- 2020-04-16
Published in:
- Nature catalysis. - 2020
English
A worldwide replacement of the toxic mercuric chloride catalyst in vinyl chloride manufacture via acetylene hydrochlorination is slowed down by the limited durability of alternative catalytic systems at high space velocities. Here, we demonstrate that platinum single atoms on carbon carriers are substantially more stable (up to 1073 K) than their gold counterparts (up to 473 K), enabling facile and scalable preparation and precise tuning of their coordination environment by simple temperature control. By combining kinetic analysis, advanced characterisation, and density functional theory, we assess how the Pt species determines the catalytic performance and thereby identify Pt(II)-Cl as the active site, being three times more active than Pt nanoparticles. Remarkably, we show that Pt single atoms exhibit outstanding stability in acetylene hydrochlorination and surpass the space-time-yields of their gold-based analogues after 25 h time-on-stream, qualifying as candidate for sustainable vinyl chloride production.
- Language
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- English
- Open access status
- green
- Identifiers
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- DOI 10.1038/s41929-020-0431-3
- PMID 32292878
- Persistent URL
- https://folia.unifr.ch/global/documents/159092
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