Oxidative dehydrogenation of ethane over alumina-supported Pd catalysts. Effect of alumina overlayer

Baosong Fu, Junling Lu, Peter C Stair, Guomin Xiao, Mayfair C. Kung, Harold H Kung

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

The effect a 45 atom-thick overlayer of aluminum oxide, deposited by atomic layer deposition, was investigated on a 2.5 wt.% Pd/Al2O3 catalyst in which the Pd nanoparticles were encapsulated by the support consequent to the preparation method. The overlayer suppressed the activity for oxidative dehydrogenation of ethane, but it also effectively prevented metal sintering and suppressed coking for reactions at high temperatures. On the catalyst with the alumina overlayer, a steady activity was observed even at 600 °C and above when the gaseous oxygen was completely consumed, while attaining 70% selectivity for ethene at 38% conversion, versus 10% selectivity at comparable conversions without the overlayer. The overlayer preferentially deposited on edge Pd atoms, as indicated by preferentially suppression of the CO chemisorption peak at 2056 cm-1, which are responsible for coking. The high ethene selectivity at 675 °C could be due to coupled homogeneous and heterogeneous reactions at the high temperature, together with phase change of PdO to Pd.

Original languageEnglish
Pages (from-to)289-295
Number of pages7
JournalJournal of Catalysis
Volume297
DOIs
Publication statusPublished - Jan 2013

Fingerprint

Ethane
Aluminum Oxide
Coking
Dehydrogenation
dehydrogenation
Catalyst supports
ethane
Alumina
aluminum oxides
selectivity
catalysts
Atoms
Catalysts
Atomic layer deposition
Carbon Monoxide
Chemisorption
Sintering
Metals
Oxygen
atomic layer epitaxy

Keywords

  • Alumina overlayer
  • Ethane
  • Oxidative dehydrogenation
  • Pd catalyst

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

Oxidative dehydrogenation of ethane over alumina-supported Pd catalysts. Effect of alumina overlayer. / Fu, Baosong; Lu, Junling; Stair, Peter C; Xiao, Guomin; Kung, Mayfair C.; Kung, Harold H.

In: Journal of Catalysis, Vol. 297, 01.2013, p. 289-295.

Research output: Contribution to journalArticle

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AU - Lu, Junling

AU - Stair, Peter C

AU - Xiao, Guomin

AU - Kung, Mayfair C.

AU - Kung, Harold H

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N2 - The effect a 45 atom-thick overlayer of aluminum oxide, deposited by atomic layer deposition, was investigated on a 2.5 wt.% Pd/Al2O3 catalyst in which the Pd nanoparticles were encapsulated by the support consequent to the preparation method. The overlayer suppressed the activity for oxidative dehydrogenation of ethane, but it also effectively prevented metal sintering and suppressed coking for reactions at high temperatures. On the catalyst with the alumina overlayer, a steady activity was observed even at 600 °C and above when the gaseous oxygen was completely consumed, while attaining 70% selectivity for ethene at 38% conversion, versus 10% selectivity at comparable conversions without the overlayer. The overlayer preferentially deposited on edge Pd atoms, as indicated by preferentially suppression of the CO chemisorption peak at 2056 cm-1, which are responsible for coking. The high ethene selectivity at 675 °C could be due to coupled homogeneous and heterogeneous reactions at the high temperature, together with phase change of PdO to Pd.

AB - The effect a 45 atom-thick overlayer of aluminum oxide, deposited by atomic layer deposition, was investigated on a 2.5 wt.% Pd/Al2O3 catalyst in which the Pd nanoparticles were encapsulated by the support consequent to the preparation method. The overlayer suppressed the activity for oxidative dehydrogenation of ethane, but it also effectively prevented metal sintering and suppressed coking for reactions at high temperatures. On the catalyst with the alumina overlayer, a steady activity was observed even at 600 °C and above when the gaseous oxygen was completely consumed, while attaining 70% selectivity for ethene at 38% conversion, versus 10% selectivity at comparable conversions without the overlayer. The overlayer preferentially deposited on edge Pd atoms, as indicated by preferentially suppression of the CO chemisorption peak at 2056 cm-1, which are responsible for coking. The high ethene selectivity at 675 °C could be due to coupled homogeneous and heterogeneous reactions at the high temperature, together with phase change of PdO to Pd.

KW - Alumina overlayer

KW - Ethane

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