Synergistic Effects in Bimetallic Palladium-Copper Catalysts Improve Selectivity in Oxygenate Coupling Reactions

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Date

2016-06-01

Author

Goulas, Konstantinos A.
SREEKUMAR, Sanil
Song, Yuying
Kharidehal, Purnima
Günbaş, Emrullah Görkem
Dietrich, Paul J.
Johnson, Gregory R.
Wang, Y. C.
Grippo, Adam M.
Grabow, Lars C.
Gokhale, Amit A.
Toste, F. Dean

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Condensation reactions such as Guerbet and aldol are important since they allow for C-C bond formation and give higher molecular weight oxygenates. An initial study identified Pd-supported on hydrotalcite as an active catalyst for the, transformation, although this catalyst showed extensive undesirable decarbonylation. A catalyst containing Pd and Cu in a 3:1 ratio dramatically decreased decarbonylation, while preserving the high catalytic rates seen with Pd-based catalysts. A combination of XRD, EXAFS, TEM, and CO chemisorption and TPD revealed the formation of CuPd bimetallic nanoparticles with a Cu-enriched surface. Finally, density functional theory studies suggest that the surface segregation of Cu atoms in the bimetallic alloy catalyst produces Cu sites with increased reactivity, while the Pd sites responsible for unselective decarbonylation pathways are selectively poisoned by CO.

Subject Keywords

Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis

URI

https://hdl.handle.net/11511/38941

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

DOI

https://doi.org/10.1021/jacs.6b02247

Collections

Department of Chemistry, Article

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Citation Formats

K. A. Goulas et al., “Synergistic Effects in Bimetallic Palladium-Copper Catalysts Improve Selectivity in Oxygenate Coupling Reactions,” JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, pp. 6805–6812, 2016, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/38941.