Blurring the boundary between homogenous and heterogeneous catalysis using palladium nanoclusters with dynamic surfaces

Israel Cano, Andreas Weilhard, Carmen Martin, Jose Pinto, Rhys W. Lodge, Ana R. Santos, Graham A. Rance, Elina Harriet Åhlgren, Erlendur Jónsson, Jun Yuan, Ziyou Y. Li, Peter Licence, Andrei N. Khlobystov and Jesum Alves Fernandes ()
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Israel Cano: University of Nottingham
Andreas Weilhard: University of Nottingham
Carmen Martin: University of Nottingham
Jose Pinto: University of Nottingham
Rhys W. Lodge: University of Nottingham
Ana R. Santos: University of Nottingham
Graham A. Rance: University of Nottingham
Elina Harriet Åhlgren: University of Nottingham
Erlendur Jónsson: University of Cambridge
Jun Yuan: University of York
Ziyou Y. Li: University of Birmingham
Peter Licence: University of Nottingham
Andrei N. Khlobystov: University of Nottingham
Jesum Alves Fernandes: University of Nottingham

Nature Communications, 2021, vol. 12, issue 1, 1-6

Abstract: Abstract Using a magnetron sputtering approach that allows size-controlled formation of nanoclusters, we have created palladium nanoclusters that combine the features of both heterogeneous and homogeneous catalysts. Here we report the atomic structures and electronic environments of a series of metal nanoclusters in ionic liquids at different stages of formation, leading to the discovery of Pd nanoclusters with a core of ca. 2 nm surrounded by a diffuse dynamic shell of atoms in [C4C1Im][NTf2]. Comparison of the catalytic activity of Pd nanoclusters in alkene cyclopropanation reveals that the atomically dynamic surface is critically important, increasing the activity by a factor of ca. 2 when compared to compact nanoclusters of similar size. Catalyst poisoning tests using mercury and dibenzo[a,e]cyclooctene show that dynamic Pd nanoclusters maintain their catalytic activity, which demonstrate their combined features of homogeneous and heterogeneous catalysts within the same material. Additionally, kinetic studies of cyclopropanation of alkenes mediated by the dynamic Pd nanoclusters reveal an observed catalyst order of 1, underpinning the pseudo-homogeneous character of the dynamic Pd nanoclusters.

Date: 2021
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DOI: 10.1038/s41467-021-25263-6

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