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Title: Dry reforming of methane over CeO2-supported Pt-Co catalysts with enhanced activity

Journal Article · · Applied Catalysis. B, Environmental
 [1];  [2];  [3];  [4];  [3];  [5];  [3];  [4];  [3];  [6];  [7];  [8]
  1. Chongqing Univ., Chongqing (China). College of Power Engineering; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Tsinghua Univ., Beijing (China). Dept. of Chemical Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
  4. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
  5. Stony Brook Univ., NY (United States). Material Science and Engineering
  6. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS). X-ray Science Division
  7. Chongqing Univ., Chongqing (China). College of Power Engineering
  8. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
SC0012704; AC02-06CH11357; AC02-05CH11231; 16-045; 21673125
OSTI ID:
1466584
Alternate ID(s):
OSTI ID: 1481171; OSTI ID: 1591652
Report Number(s):
BNL-207986-2018-JAAM
Journal Information:
Applied Catalysis. B, Environmental, Vol. 236, Issue C; ISSN 0926-3373
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 88 works
Citation information provided by
Web of Science

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