Dry Reforming of Ethane and Butane with CO₂ over PtNi/CeO₂ Bimetallic Catalysts

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Abstract

Dry reforming is a potential process to convert CO2 and light alkanes into syngas (H2 and CO), which can be subsequently transformed to chemicals and fuels. In this work, PtNi bimetallic catalysts have been investigated for dry reforming of ethane and butane using both model surfaces and supported powder catalysts. The PtNi bimetallic catalyst shows an improvement in both activity and stability in comparison to the corresponding monometallic catalysts. The formation of PtNi alloy and the partial reduction of Ce4+ to Ce3+ under reaction conditions are demonstrated by in situ ambient-pressure X-ray photoemission spectroscopy (AP-XPS), X-ray diffraction (XRD), and X-ray absorption fine structure (XAFS) measurements. A Pt-rich bimetallic surface is revealed by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) following CO adsorption. Combined in situ experimental results and density functional theory (DFT) calculations suggest that the Pt-rich PtNi bimetallic surface structure would weaken the binding of surface oxygenate/carbon species and reduce the activation energy for C–C bond scission, leading to an enhanced dry reforming activity.

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