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Title: Dry reforming of methane over CeO 2-supported Pt-Co catalysts with enhanced activity

Abstract

Dry reforming of methane provides opportunities of using CH 4 and CO 2 to produce syngas. The PtCo/CeO 2 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/CeO 2 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/CeO 2 promotes CH 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/CeO 2 catalyst is resistant to coke formation as effectively as Pt/CeO 2 and can be easily regenerated by a mild CO 2 treatment.

Authors:
 [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
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) (SC-22). Scientific User Facilities Division; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1466584
Alternate Identifier(s):
OSTI ID: 1481171
Report Number(s):
BNL-207986-2018-JAAM
Journal ID: ISSN 0926-3373
Grant/Contract Number:  
SC0012704; AC02-06CH11357
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.
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.
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.
@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 H2/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 CH 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}
}

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