Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 236, Issue -, Pages 280-293Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2018.05.035
Keywords
Dry reforming of methane (DRM); Pt-Co; Kinetics; Density functional theory (DFT); Regeneration
Funding
- U.S. Department of Energy (DOE) [DE-AC02-98CH10886 with]
- Brookhaven National Laboratory Directed Research and Development (LDRD) Project [16-045]
- National Natural Science Foundation of China (NSFC) [21673125]
- China Scholarship Council
- Tang Lixin Scholarship
- Office of Science of the DOE [DE-AC02-05CH11231]
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Dry reforming of methane provides opportunities of using CH4 and CO2 to produce syngas. The PtCo/CeO2 bimetallic catalyst shows higher activity and H-2/CO ratio than the corresponding monometallic catalysts, mainly attributed to the synergistic effect of Pt-Co. Structural feature of the PtCo/CeO2 catalyst was revealed by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of adsorbed CO and in situ techniques like X-ray diffraction (XRD), X-ray adsorption fine structure (XAFS) and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS). Pt-Co alloy and separated Co particles co-existed in the bimetallic catalyst, whereas the former was determined as the dominant active structure with a Pt-Co-mixed-surface termination. During reaction, Pt and Co in the alloy structure nearly maintained their metallic state with slight oxygen decoration, yielding oxygen-metal site-pairs (O*-*). Combined kinetic investigations and DFT calculations reveal that the O*-modified catalytic surface of PtCo/CeO2 promotes C-H bond activation with higher entropy contribution (less constraints) to compensate its higher activation barrier. Thermogravimetric analysis (TGA), transmission electron microscope (TEM) and Raman spectroscopy show that the PtCo/CeO2 catalyst is resistant to coke formation as effectively as Pt/CeO2 and can be easily regenerated by a mild CO2 treatment.
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