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Title: Comparative study of carbon dioxide reforming of methane to synthesis gas over Ni/La{sub 2}O{sub 3} and conventional nickel-based catalysts

Journal Article · · Journal of Physical Chemistry
DOI:https://doi.org/10.1021/jp951809e· OSTI ID:196648
;  [1]; ;  [2]
  1. Univ. of Patras (Greece)
  2. Univ. of Strathclyde, Glasgow (United Kingdom)

Carbon dioxide reforming of methane to synthesis gas was studied by employing a Ni/La{sub 2}O{sub 3} catalyst as well as conventional nickel-based catalysts, i.e., Ni/{gamma}-Al{sub 2}O{sub 3}, Ni/CaO/{gamma}-Al{sub 2}O{sub 3}, and Ni/CaO. It is observed that, in constrast to conventional nickel-based catalysts, which exhibit continuous deactivation with time on stream, the rate of reaction over the Ni/La{sub 2}O{sub 3} catalyst increase during the initial 2-5 h and then tends to be essentially invariable with time on stream. X-ray photoelectron spectroscopy (XPS) studies show that the surface carbon on spent Ni/Al{sub 2}O{sub 3} catalyst is dominated by -C-C- species that eventually block the entire Ni surface, leading to total loss of activity. The surface carbon on the working Ni/La{sub 2}O{sub 3} catalyst is found to consist of -C-C- species and a large amount of oxidized carbon. Both XPS and secondary ion mass spectrometry results reveal that a large fraction of surface Ni on the working Ni/La{sub 2}O{sub 3} catalyst is not shielded by carbon deposition. FTIR studies reveal that the enhancement of the rate of reaction over the Ni/La{sub 2}O{sub 3} catalyst during the initial 2-5 h of reaction correlates well with increasing concentrations of La{sub 2}O{sub 2}CO{sub 3} and formate species on the support, suggesting that these species may participate in the surface chemistry to produce synthesis gas. 47 refs., 12 figs., 2 tabs.

OSTI ID:
196648
Journal Information:
Journal of Physical Chemistry, Vol. 100, Issue 2; Other Information: PBD: 11 Jan 1996
Country of Publication:
United States
Language:
English