Unlocking synergy in bimetallic catalysts by core–shell design

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Extending the toolbox from mono- to bimetallic catalysts is key in realizing efficient chemical processes1. Traditionally, the performance of bimetallic catalysts featuring one active and one selective metal is optimized by varying the metal composition1–3, often resulting in a compromise between the catalytic properties of the two metals4–6. Here we show that by designing the atomic distribution of bimetallic Au–Pd nanocatalysts, we obtain a synergistic catalytic performance in the industrially relevant selective hydrogenation of butadiene. Our single-crystalline Au-core Pd-shell nanorods were up to 50 times more active than their alloyed and monometallic counterparts, while retaining high selectivity. We find a shell-thickness-dependent catalytic activity, indicating that not only the nature of the surface but also several subsurface layers play a crucial role in the catalytic performance, and rationalize this finding using density functional theory calculations. Our results open up an alternative avenue for the structural design of bimetallic catalysts.

Original languageEnglish
Pages (from-to)1216-1220
Number of pages5
JournalNature Materials
Volume20
Issue number9
DOIs
Publication statusPublished - Sept 2021

Bibliographical note

Funding Information:
We thank R. Beerthuis and J.W. de Rijk for useful discussions and technical support. We thank N. Masoud for providing the gold catalyst reference data. We thank S. Dussi for critically reading the manuscript. We thank S. Zanoni for useful discussions regarding the carbon monoxide infrared spectroscopy measurements. This project received funding from the European Research Council under the European Union’s Horizon 2020 research and innovation programme (ERC-2014-CoG no. 648991) and the European Union’s Seventh Framework Programme (FP-2007-2013; European Research Council Advanced Grant Agreement #291667 HierarSACol). J.E.S.v.d.H. also acknowledges the graduate programme of the Debye Institute for Nanomaterials Science (Utrecht University), which is facilitated by grant 022.004.016 of the Netherlands Organisation for Scientific Research. J.J. and F.S. gratefully acknowledge support by the state of Baden-Württemberg through bwHPC (bwunicluster and JUSTUS, RV bw17D011) as well as financial support from the Helmholtz Association.

Publisher Copyright:
© 2021, The Author(s), under exclusive licence to Springer Nature Limited.

Funding

We thank R. Beerthuis and J.W. de Rijk for useful discussions and technical support. We thank N. Masoud for providing the gold catalyst reference data. We thank S. Dussi for critically reading the manuscript. We thank S. Zanoni for useful discussions regarding the carbon monoxide infrared spectroscopy measurements. This project received funding from the European Research Council under the European Union’s Horizon 2020 research and innovation programme (ERC-2014-CoG no. 648991) and the European Union’s Seventh Framework Programme (FP-2007-2013; European Research Council Advanced Grant Agreement #291667 HierarSACol). J.E.S.v.d.H. also acknowledges the graduate programme of the Debye Institute for Nanomaterials Science (Utrecht University), which is facilitated by grant 022.004.016 of the Netherlands Organisation for Scientific Research. J.J. and F.S. gratefully acknowledge support by the state of Baden-Württemberg through bwHPC (bwunicluster and JUSTUS, RV bw17D011) as well as financial support from the Helmholtz Association.

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