Improving Catalytic Stability and Coke Resistance of Ni/Al₂O₃ Catalysts with Ce Promoter for Relatively Low Temperature Dry Reforming of Methane Reaction

Abstract

A series of Ni catalysts supported on alumina with different Ce contents(1.0%–6.0%, mass fraction) was prepared by the impregnation method and used for dry reforming of methane(DRM) at a relatively low temperature of 650 °C. The promotion effect of Ce with different loading amounts on the physicochemical properties of the catalysts was systematically characterized by transmission electron microscopy(TEM), X-ray diffraction(XRD), N₂ adsorption-desorption, thermo elemental IRIS Intrepid inductively coupled plasma atomic emission spectrometer (ICP-AES), UV-visible diffuse reflectance spectroscopy(UV-Vis DRS), Fourier transformation infrared(FTIR) spectra, H2-temperature programmed reduction(H₂-TPR) analysis, H2-temperature programmed desorption(H₂-TPD), and The X-ray photoelectron spectroscopy(XPS) techniques. The results indicate that all the catalysts mainly exist in the NiAl₂O₄ phase after being calcined at 750 °C with small Ni particle sizes due to the strong metal-support interaction derived from the reduction of the NiAl₂O₄ phase. The Ce-promoted catalysts show better catalytic performance as well as the resistance against sintering of Ni particles and deposition of carbon compared to the Ni/Al₂O₃ catalyst. The Ni-6Ce/Al₂O₃ exhibits the best catalytic stability and coke resistance among the four catalysts studied, which is due to its small Ni nanoparticles sizes, excellent reducibility as well as high amount of active oxygen species. In a 400 h stability test for DRM reaction at 650 °C, Ni-6Ce/Al₂O₃ exhibits less coke deposition and small growth of Ni nanoparticles. This work provides a simple way to preparing the Ni-Ce/Al₂O₃ catalyst with enhanced catalytic performance in DRM. The Ni-6Ce/Al₂O₃ catalyst has great potential for industrial application due to its anti-sintering ability and resistance to carbon deposition.

Keywords

Dry reforming of methane(DRM) / Cerium oxide / Ni-based catalyst / Coke resistance

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