Dry reforming of methane (DRM) utilizes two abundantly available greenhouse gases to produce industrially important syngas. Syngas is used to produce synthetic petroleum as fuels or chemicals. The conversion of methane, the primary component of natural gas, to higher value products will become increasingly important for the near future. Current global challenge for the DRM reaction is to develop thermally stable and active catalysts that can show good resistance to deactivation. In our study, Ce1-xTixO2-y (x: 0.1, 0.2, 0.3, and 0.5) supported nickel catalysts were synthesized by sol-gel methods with controlled Ni loadings between 1 and 10 wt%. Ceria exhibits unique redox properties and oxygen storage capacities, which can better anchor Ni as small clusters and inhibit coke formation. Introduction of metal dopant, Ti, into ceria could promote its redox properties as well as enhance its thermal stability at high temperatures. All the prepared catalysts were characterized by a combination of spectroscopy and microscopy techniques including x-ray diffraction, transmission electron microscopy, scanning electron microscopy-energy dispersive spectroscopy, x-ray photoelectron spectroscopy, BET surface area, H2-chemisorption, and H2-temperature-programmed reduction. The DRM performance was investigated in a continuous gas flow reactor using gas chromatography and mass spectrometry instruments and compared with respect to reaction temperatures, Ce:Ti ratios in the oxide supports, and Ni loadings. Our data show the formation of Ce1-xTixO2-y solid mixed oxide supports. The 2 wt.% Ni/Ce0.7Ti0.3O2-y catalyst was identified to deliver excellent catalytic activity and stability (up to 50 h) during the DRM reaction on stream among all the ceria supports and Ni loadings examined. The enhanced reactivity and stability of this catalyst can be attributed to the unique interaction between the Ni metal and Ce0.7Ti0.3O2-y support. Additionally, we compared the dry reforming of methane activity over 2 wt.% Ni/Ce0.7Ti0.3O2-y catalysts to the reforming of propane and ethane.

Dry reforming of methane over nickel/Ti-doped ceria catalysts

2019 Fall National Meeting

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