Au–Pd separation enhances bimetallic catalysis of alcohol oxidation

Xiaoyang Huang, Ouardia Akdim, Mark Douthwaite, Kai Wang, Liang Zhao, Richard J. Lewis, Samuel Pattisson, Isaac T. Daniel, Peter J. Miedziak, Greg Shaw, David J. Morgan, Sultan M. Althahban, Thomas E. Davies, Qian He, Fei Wang, Jile Fu, Donald Bethell, Steven McIntosh, Christopher J. Kiely and Graham J. Hutchings ()
Additional contact information
Xiaoyang Huang: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Ouardia Akdim: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Mark Douthwaite: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Kai Wang: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Liang Zhao: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Richard J. Lewis: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Samuel Pattisson: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Isaac T. Daniel: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Peter J. Miedziak: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Greg Shaw: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
David J. Morgan: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Sultan M. Althahban: Lehigh University
Thomas E. Davies: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Qian He: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Fei Wang: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Jile Fu: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Donald Bethell: Cardiff Catalysis Institute, School of Chemistry, Cardiff University
Steven McIntosh: Lehigh University
Christopher J. Kiely: Lehigh University
Graham J. Hutchings: Cardiff Catalysis Institute, School of Chemistry, Cardiff University

Nature, 2022, vol. 603, issue 7900, 271-275

Abstract: Abstract In oxidation reactions catalysed by supported metal nanoparticles with oxygen as the terminal oxidant, the rate of the oxygen reduction can be a limiting factor. This is exemplified by the oxidative dehydrogenation of alcohols, an important class of reactions with modern commercial applications1–3. Supported gold nanoparticles are highly active for the dehydrogenation of the alcohol to an aldehyde4 but are less effective for oxygen reduction5,6. By contrast, supported palladium nanoparticles offer high efficacy for oxygen reduction5,6. This imbalance can be overcome by alloying gold with palladium, which gives enhanced activity to both reactions7,8,9; however, the electrochemical potential of the alloy is a compromise between that of the two metals, meaning that although the oxygen reduction can be improved in the alloy, the dehydrogenation activity is often limited. Here we show that by separating the gold and palladium components in bimetallic carbon-supported catalysts, we can almost double the reaction rate compared with that achieved with the corresponding alloy catalyst. We demonstrate this using physical mixtures of carbon-supported monometallic gold and palladium catalysts and a bimetallic catalyst comprising separated gold and palladium regions. Furthermore, we demonstrate electrochemically that this enhancement is attributable to the coupling of separate redox processes occurring at isolated gold and palladium sites. The discovery of this catalytic effect—a cooperative redox enhancement—offers an approach to the design of multicomponent heterogeneous catalysts.

Date: 2022
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DOI: 10.1038/s41586-022-04397-7

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