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UnlockingSynergy_JvdH.pdf (8.16 MB)

Unlocking Synergy in Bimetallic Catalysts by Core-Shell Design

preprint
submitted on 10.11.2020, 22:37 and posted on 12.11.2020, 12:56 by Jessi van der Hoeven, Jelena Jelic, Liselotte Olthof, Giorgio Totarella, Relinde J. A. van Dijk-Moes, Felix Studt, Alfons Van Blaaderen, Petra E. de Jongh
Extending the toolbox from mono- to bimetallic catalysts is key in realizing efficient chemical processes. Traditionally, the performance of bimetallic catalysts featuring one active and one selective metal is optimized by varying the metal composition, often resulting in a compromise between the catalytic properties of the two metals. 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 sub-surface layers play a crucial role in the catalytic performance, and rationalize this finding using density-functional-theory calculations. Our results open up a novel avenue for the structural design of bimetallic catalysts.

Funding

ERC-2014-CoG No 648991

ERC Advanced Grant Agreement #291667 HierarSACol

NWO grant 022.004.016

bwHPC (bwunicluster and JUSTUS, RV bw17D011)

History

Email Address of Submitting Author

j.e.s.vanderhoeven@uu.nl

Institution

Utrecht University

Country

Netherlands

ORCID For Submitting Author

0000-0001-9832-289X

Declaration of Conflict of Interest

The authors declare no competing interests

Version Notes

Supporting information available upon request

Exports