skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Abstract

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.

Authors:
 [1];  [2];  [3];  [4];  [3];  [5];  [3];  [4];  [3];  [6];  [7];  [8]
+ Show Author Affiliations
  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
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1466584
Alternate Identifier(s):
OSTI ID: 1481171; OSTI ID: 1591652
Report Number(s):
BNL-207986-2018-JAAM
Journal ID: ISSN 0926-3373
Grant/Contract Number:  
SC0012704; AC02-06CH11357; AC02-98CH10886; 16-045; AC02-76SF00515; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Applied Catalysis B: Environmental
Additional Journal Information:
Journal Volume: 236; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Dry reforming of methane (DRM); Pt-Co; Kinetics; Density functional theory (DFT); Regeneration; Density functional theory; Dry reforming of methane

Citation Formats

Xie, Zhenhua, Yan, Binhang, Kattel, Shyam, Lee, Ji Hoon, Yao, Siyu, Wu, Qiyuan, Rui, Ning, Gomez, Elaine, Liu, Zongyuan, Xu, Wenqian, Zhang, Li, and Chen, Jingguang G. Dry reforming of methane over CeO2-supported Pt-Co catalysts with enhanced activity. United States: N. p., 2018. Web. doi:10.1016/j.apcatb.2018.05.035.
Copy to clipboard
Xie, Zhenhua, Yan, Binhang, Kattel, Shyam, Lee, Ji Hoon, Yao, Siyu, Wu, Qiyuan, Rui, Ning, Gomez, Elaine, Liu, Zongyuan, Xu, Wenqian, Zhang, Li, & Chen, Jingguang G. Dry reforming of methane over CeO2-supported Pt-Co catalysts with enhanced activity. United States. doi:10.1016/j.apcatb.2018.05.035.
Copy to clipboard
Xie, Zhenhua, Yan, Binhang, Kattel, Shyam, Lee, Ji Hoon, Yao, Siyu, Wu, Qiyuan, Rui, Ning, Gomez, Elaine, Liu, Zongyuan, Xu, Wenqian, Zhang, Li, and Chen, Jingguang G. Sat . "Dry reforming of methane over CeO2-supported Pt-Co catalysts with enhanced activity". United States. doi:10.1016/j.apcatb.2018.05.035. https://www.osti.gov/servlets/purl/1466584.
Copy to clipboard
@article{osti_1466584,
title = {Dry reforming of methane over CeO2-supported Pt-Co catalysts with enhanced activity},
author = {Xie, Zhenhua and Yan, Binhang and Kattel, Shyam and Lee, Ji Hoon and Yao, Siyu and Wu, Qiyuan and Rui, Ning and Gomez, Elaine and Liu, Zongyuan and Xu, Wenqian and Zhang, Li and Chen, Jingguang G.},
abstractNote = {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.},
doi = {10.1016/j.apcatb.2018.05.035},
journal = {Applied Catalysis B: Environmental},
number = C,
volume = 236,
place = {United States},
year = {2018},
month = {5}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI:  10.1016/j.apcatb.2018.05.035
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referencing / citing this record:

Influence of Solid Solution Formation on the Activity of CeO2 Supported Ni–Cu Mixed Oxide Catalysts in Dry Reforming of Methane
journal, May 2019

Atomically dispersed nickel as coke-resistant active sites for methane dry reforming
journal, November 2019

A highly efficient 2D siloxene coated Ni foam catalyst for methane dry reforming and an effective approach to recycle the spent catalyst for energy storage applications
journal, January 2019

  • Krishnamoorthy, Karthikeyan; M. S. P., Sudhakaran; Pazhamalai, Parthiban
  • Journal of Materials Chemistry A, Vol. 7, Issue 32
  • DOI: 10.1039/c9ta03584b
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: