Nanoengineering the active site in heterogeneous catalysis

A.F. Lee, C.V. Ellis, M.A. Newton, C.M.A. Parlett, K. Wilson

Research output: Contribution to journalMeeting abstract

Abstract

Here we demonstrate the first application of time-resolved synchrotron X-ray absorption spectroscopy to simultaneously follow dynamic nanoparticle surface restructuring and the evolution of surface and gas-phase products during an organic reaction. Surface palladium oxide, and not metal, is identified as the catalytic species responsible for the selective oxidation (selox) of crotyl alcohol to crotonaldehyde. Elevated reaction temperatures facilitate reversible nanoparticle redox processes, and concomitant catalytic selectivity loss, in response to reaction conditions. These discoveries highlight the importance of stabilizing surface palladium oxide and minimizing catalyst reducibility in order to achieve high selox yields, and will aid the future design of Pd-derived selox catalysts. This discovery has important implications for the design of future liquid and vapor phase selox catalysts, and the thermochemical behavior of Pd nanostructures in general.
Original languageEnglish
Number of pages1
JournalAbstracts of Papers of the American Chemical Society
Publication statusPublished - 2011
Event242nd ACS National Meeting and Exposition - Denver, CO, United States
Duration: 28 Aug 20111 Sep 2011

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Catalysis
Oxidation
2-butenal
Palladium
Catalysts
Nanoparticles
X ray absorption spectroscopy
Oxides
Synchrotrons
Nanostructures
Alcohols
Gases
Metals
Vapors
Liquids
Temperature
palladium oxide

Bibliographical note

242nd ACS National Meeting and Exposition; Denver, CO; United States; 28 August 2011 through 1 September 2011

Cite this

Lee, A. F., Ellis, C. V., Newton, M. A., Parlett, C. M. A., & Wilson, K. (2011). Nanoengineering the active site in heterogeneous catalysis. Abstracts of Papers of the American Chemical Society.
Lee, A.F. ; Ellis, C.V. ; Newton, M.A. ; Parlett, C.M.A. ; Wilson, K. / Nanoengineering the active site in heterogeneous catalysis. In: Abstracts of Papers of the American Chemical Society. 2011.
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Nanoengineering the active site in heterogeneous catalysis. / Lee, A.F.; Ellis, C.V.; Newton, M.A.; Parlett, C.M.A.; Wilson, K.

In: Abstracts of Papers of the American Chemical Society, 2011.

Research output: Contribution to journalMeeting abstract

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AU - Lee, A.F.

AU - Ellis, C.V.

AU - Newton, M.A.

AU - Parlett, C.M.A.

AU - Wilson, K.

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AB - Here we demonstrate the first application of time-resolved synchrotron X-ray absorption spectroscopy to simultaneously follow dynamic nanoparticle surface restructuring and the evolution of surface and gas-phase products during an organic reaction. Surface palladium oxide, and not metal, is identified as the catalytic species responsible for the selective oxidation (selox) of crotyl alcohol to crotonaldehyde. Elevated reaction temperatures facilitate reversible nanoparticle redox processes, and concomitant catalytic selectivity loss, in response to reaction conditions. These discoveries highlight the importance of stabilizing surface palladium oxide and minimizing catalyst reducibility in order to achieve high selox yields, and will aid the future design of Pd-derived selox catalysts. This discovery has important implications for the design of future liquid and vapor phase selox catalysts, and the thermochemical behavior of Pd nanostructures in general.

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