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Title: Dry Reforming of Ethane and Butane with CO 2 over PtNi/CeO 2 Bimetallic Catalysts

Dry reforming is a potential process to convert CO 2 and light alkanes into syngas (H 2 and CO), which can be subsequently transformed to chemicals and fuels. Here 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 as compared to the corresponding monometallic catalysts. The formation of PtNi alloy and the partial reduction of Ce 4+ to Ce 3+ 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 oxygenates/carbon species and reduce the activation energy for C-C bond scission, leading to an enhanced dry reforming activity.
Authors:
 [1] ;  [2] ;  [2] ;  [3] ;  [4] ;  [4] ;  [4] ;  [2] ;  [2] ;  [5]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Tsinghua Univ., Beijing (China). Dept. of Chemical Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
  3. Tsinghua Univ., Beijing (China). College of Materials Science and Engineering
  4. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Publication Date:
Report Number(s):
BNL-113425-2017-JA
Journal ID: ISSN 2155-5435; R&D Project: CO035; KC0302010; TRN: US1701623
Grant/Contract Number:
SC0012704; AC02-98CH10886; FG02-05ER15688; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 11; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; dry reforming; bimetallic catalyst; synthesis gas; ethane; butane; CO2
OSTI Identifier:
1342631

Yan, Binhang, Yang, Xiaofang, Yao, Siyu, Wan, Jie, Myint, MyatNoeZin, Gomez, Elaine, Xie, Zhenhua, Kattel, Shyam, Xu, Wenqian, and Chen, Jingguang G. Dry Reforming of Ethane and Butane with CO2 over PtNi/CeO2 Bimetallic Catalysts. United States: N. p., Web. doi:10.1021/acscatal.6b02176.
Yan, Binhang, Yang, Xiaofang, Yao, Siyu, Wan, Jie, Myint, MyatNoeZin, Gomez, Elaine, Xie, Zhenhua, Kattel, Shyam, Xu, Wenqian, & Chen, Jingguang G. Dry Reforming of Ethane and Butane with CO2 over PtNi/CeO2 Bimetallic Catalysts. United States. doi:10.1021/acscatal.6b02176.
Yan, Binhang, Yang, Xiaofang, Yao, Siyu, Wan, Jie, Myint, MyatNoeZin, Gomez, Elaine, Xie, Zhenhua, Kattel, Shyam, Xu, Wenqian, and Chen, Jingguang G. 2016. "Dry Reforming of Ethane and Butane with CO2 over PtNi/CeO2 Bimetallic Catalysts". United States. doi:10.1021/acscatal.6b02176. https://www.osti.gov/servlets/purl/1342631.
@article{osti_1342631,
title = {Dry Reforming of Ethane and Butane with CO2 over PtNi/CeO2 Bimetallic Catalysts},
author = {Yan, Binhang and Yang, Xiaofang and Yao, Siyu and Wan, Jie and Myint, MyatNoeZin and Gomez, Elaine and Xie, Zhenhua and Kattel, Shyam and Xu, Wenqian and Chen, Jingguang G.},
abstractNote = {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. Here 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 as compared 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 oxygenates/carbon species and reduce the activation energy for C-C bond scission, leading to an enhanced dry reforming activity.},
doi = {10.1021/acscatal.6b02176},
journal = {ACS Catalysis},
number = 11,
volume = 6,
place = {United States},
year = {2016},
month = {9}
}