Structure and reactivity investigations on supported bimetallic Au{single bond}Ni catalysts used for hydrocarbon steam reforming

Ya Huei (Cathy) Chin, David L. King, Hyunseog Roh, Yong Wang, Steven M. Heald

Research output: Contribution to journalArticle

112 Citations (Scopus)

Abstract

The addition of small quantities of gold to the surface of supported nickel catalysts has been described as a means to retard carbon formation during hydrocarbon steam reforming. Calculations by others have indicated that gold locates at the most catalytically active (step and edge) sites that also serve as nucleation sites for carbon formation. In this paper, we describe experiments to characterize the Ni{single bond}Au interactions on bimetallic Au{single bond}Ni/MgAl2O4 catalysts at various Ni and Au loadings. The catalyst structure was investigated using EXAFS/XANES spectroscopy and adsorption-desorption measurements with H2 and N2O. Evidence for surface alloy formation is provided in the Ni K-edge and Au LIII-edge EXAFS measurements of Au-promoted 8.8% Ni/MgAl2O4, especially at Au loadings ≤ 0.2   wt%. At higher Au concentrations, there is evidence of a combination of alloy and segregated Au species. H2 chemisorption and N2O temperature-programmed desorption (TPD) measurements showed a significant decrease in total surface sites, or surface site reactivity, on Au-modified Ni/MgAl2O4 catalyst. The XANES structure is consistent with perturbation of the electronic structure of both the Ni and Au atoms as a result of alloy formation. TGA studies with steam/n-butane feed confirmed the ability of Au to retard coke deposition under low S/C reforming conditions, although carbon formation was not fully suppressed. When testing for methane steam reforming, a lower initial activity and deactivation rate resulted from Au promotion of the Ni catalyst. However, both catalysts showed a declining activity with time. The lack of a direct correlation between the surface characterization results and catalytic activity is most likely a result of decreasing effectiveness of the surface alloy with increasing temperature.

Original languageEnglish
Pages (from-to)153-162
Number of pages10
JournalJournal of Catalysis
Volume244
Issue number2
DOIs
Publication statusPublished - 2006 Dec 10

Fingerprint

Steam reforming
Hydrocarbons
steam
reactivity
hydrocarbons
catalysts
Catalysts
Carbon
Gold
carbon
Catalyst activity
desorption
Extended X ray absorption fine structure spectroscopy
gold
X ray absorption near edge structure spectroscopy
coke
Steam
Butane
promotion
Temperature programmed desorption

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

Chin, Ya Huei (Cathy) ; King, David L. ; Roh, Hyunseog ; Wang, Yong ; Heald, Steven M. / Structure and reactivity investigations on supported bimetallic Au{single bond}Ni catalysts used for hydrocarbon steam reforming. In: Journal of Catalysis. 2006 ; Vol. 244, No. 2. pp. 153-162.
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abstract = "The addition of small quantities of gold to the surface of supported nickel catalysts has been described as a means to retard carbon formation during hydrocarbon steam reforming. Calculations by others have indicated that gold locates at the most catalytically active (step and edge) sites that also serve as nucleation sites for carbon formation. In this paper, we describe experiments to characterize the Ni{single bond}Au interactions on bimetallic Au{single bond}Ni/MgAl2O4 catalysts at various Ni and Au loadings. The catalyst structure was investigated using EXAFS/XANES spectroscopy and adsorption-desorption measurements with H2 and N2O. Evidence for surface alloy formation is provided in the Ni K-edge and Au LIII-edge EXAFS measurements of Au-promoted 8.8{\%} Ni/MgAl2O4, especially at Au loadings ≤ 0.2   wt{\%}. At higher Au concentrations, there is evidence of a combination of alloy and segregated Au species. H2 chemisorption and N2O temperature-programmed desorption (TPD) measurements showed a significant decrease in total surface sites, or surface site reactivity, on Au-modified Ni/MgAl2O4 catalyst. The XANES structure is consistent with perturbation of the electronic structure of both the Ni and Au atoms as a result of alloy formation. TGA studies with steam/n-butane feed confirmed the ability of Au to retard coke deposition under low S/C reforming conditions, although carbon formation was not fully suppressed. When testing for methane steam reforming, a lower initial activity and deactivation rate resulted from Au promotion of the Ni catalyst. However, both catalysts showed a declining activity with time. The lack of a direct correlation between the surface characterization results and catalytic activity is most likely a result of decreasing effectiveness of the surface alloy with increasing temperature.",
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Structure and reactivity investigations on supported bimetallic Au{single bond}Ni catalysts used for hydrocarbon steam reforming. / Chin, Ya Huei (Cathy); King, David L.; Roh, Hyunseog; Wang, Yong; Heald, Steven M.

In: Journal of Catalysis, Vol. 244, No. 2, 10.12.2006, p. 153-162.

Research output: Contribution to journalArticle

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