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Issue 29, 2013
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Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions

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Abstract

We report a novel synthesis of nanoparticle Pd–Cu catalysts, containing only trace amounts of Pd, for selective hydrogenation reactions. Pd–Cu nanoparticles were designed based on model single atom alloy (SAA) surfaces, in which individual, isolated Pd atoms act as sites for hydrogen uptake, dissociation, and spillover onto the surrounding Cu surface. Pd–Cu nanoparticles were prepared by addition of trace amounts of Pd (0.18 atomic (at)%) to Cu nanoparticles supported on Al2O3 by galvanic replacement (GR). The catalytic performance of the resulting materials for the partial hydrogenation of phenylacetylene was investigated at ambient temperature in a batch reactor under a head pressure of hydrogen (6.9 bar). The bimetallic Pd–Cu nanoparticles have over an order of magnitude higher activity for phenylacetylene hydrogenation when compared to their monometallic Cu counterpart, while maintaining a high selectivity to styrene over many hours at high conversion. Greater than 94% selectivity to styrene is observed at all times, which is a marked improvement when compared to monometallic Pd catalysts with the same Pd loading, at the same total conversion. X-ray photoelectron spectroscopy and UV-visible spectroscopy measurements confirm the complete uptake and alloying of Pd with Cu by GR. Scanning tunneling microscopy and thermal desorption spectroscopy of model SAA surfaces confirmed the feasibility of hydrogen spillover onto an otherwise inert Cu surface. These model studies addressed a wide range of Pd concentrations related to the bimetallic nanoparticles.

Graphical abstract: Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions

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Publication details

The article was received on 10 Apr 2013, accepted on 28 May 2013 and first published on 30 May 2013


Article type: Paper
DOI: 10.1039/C3CP51538A
Citation: Phys. Chem. Chem. Phys., 2013,15, 12187-12196
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    Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions

    M. B. Boucher, B. Zugic, G. Cladaras, J. Kammert, M. D. Marcinkowski, T. J. Lawton, E. C. H. Sykes and M. Flytzani-Stephanopoulos, Phys. Chem. Chem. Phys., 2013, 15, 12187
    DOI: 10.1039/C3CP51538A

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