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 · Thu Jan 11 04:00:00 EST 1996 · Journal of Physical Chemistry

DOI:https://doi.org/10.1021/jp951809e· OSTI ID:196648

Zhang, Z; Verykios, X E ^[1]; MacDonald, S M; Affrossman, S ^[2]

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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, Journal Name: Journal of Physical Chemistry Journal Issue: 2 Vol. 100; ISSN JPCHAX; ISSN 0022-3654
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
40 CHEMISTRY
ALUMINIUM OXIDES
BINDING ENERGY
CALCIUM OXIDES
CARBON DIOXIDE
CATALYST SUPPORTS
CATALYSTS
CATALYTIC REFORMING
INFRARED SPECTRA
LANTHANUM OXIDES
METHANE
NICKEL
PHOTOELECTRON SPECTROSCOPY
SYNTHESIS
SYNTHESIS GAS
USES