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Title: Identification of a Pt3Co Surface Intermetallic Alloy in Pt–Co Propane Dehydrogenation Catalysts

Abstract

Bimetallic Pt-Co nanoparticles (NPs) were prepared and characterized by scanning transmission electron microscopy, in situ X-ray absorption spectroscopy, in situ synchrotron X-ray diffraction, and catalytic conversion for propane dehydrogenation with and without added H-2. In addition, the surface extended X-ray absorption fine structure (EXAFS) obtained by fitting the difference spectrum between the fully reduced and room-temperature-oxidized catalysts suggest that the surface structure remains Pt3Co, although the core changes from Pt to Pt3Co and to PtCo. At low Co loading, the bimetallic nanoparticles form a Pt3Co intermetallic surface alloy with Pt-rich core. With increasing Co loading, a full alloy forms where both the surface and NP compositions are Pt3Co. A further increase in Co loading leads to a Co-rich NP core, likely PtCo, with a surface of Pt3Co. Although Pt-Co intermetallic alloys form two different phases and several morphologies, the surface structures are similar in all catalysts. Although both monometallic Pt and Co are active for alkane dehydrogenation, all bimetallic Pt-Co catalysts are significantly more olefin selective than either single metal. The turnover rates of the bimetallic catalysts indicate that Pt is the active atom with little contribution from Co atoms. The high olefin selectivity is suggested to be due tomore » Co acting as a less active structural promoter to break up large Pt ensembles in bimetallic NPs.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [1]
  1. Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; NOVA Chemicals Center for Applied Research, Calgary, Alberta (Canada)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division
  5. Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering; Dalian Univ. of Technology, Dalian, Liaoning (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division
OSTI Identifier:
1559887
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 9; Journal Issue: 6; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Cesar, Laryssa Goncalves, Yang, Ce, Lu, Zheng, Ren, Yang, Zhang, Guanghui, and Miller, Jeffrey T. Identification of a Pt3Co Surface Intermetallic Alloy in Pt–Co Propane Dehydrogenation Catalysts. United States: N. p., 2019. Web. https://doi.org/10.1021/acscatal.9b00549.
Cesar, Laryssa Goncalves, Yang, Ce, Lu, Zheng, Ren, Yang, Zhang, Guanghui, & Miller, Jeffrey T. Identification of a Pt3Co Surface Intermetallic Alloy in Pt–Co Propane Dehydrogenation Catalysts. United States. https://doi.org/10.1021/acscatal.9b00549
Cesar, Laryssa Goncalves, Yang, Ce, Lu, Zheng, Ren, Yang, Zhang, Guanghui, and Miller, Jeffrey T. Wed . "Identification of a Pt3Co Surface Intermetallic Alloy in Pt–Co Propane Dehydrogenation Catalysts". United States. https://doi.org/10.1021/acscatal.9b00549. https://www.osti.gov/servlets/purl/1559887.
@article{osti_1559887,
title = {Identification of a Pt3Co Surface Intermetallic Alloy in Pt–Co Propane Dehydrogenation Catalysts},
author = {Cesar, Laryssa Goncalves and Yang, Ce and Lu, Zheng and Ren, Yang and Zhang, Guanghui and Miller, Jeffrey T.},
abstractNote = {Bimetallic Pt-Co nanoparticles (NPs) were prepared and characterized by scanning transmission electron microscopy, in situ X-ray absorption spectroscopy, in situ synchrotron X-ray diffraction, and catalytic conversion for propane dehydrogenation with and without added H-2. In addition, the surface extended X-ray absorption fine structure (EXAFS) obtained by fitting the difference spectrum between the fully reduced and room-temperature-oxidized catalysts suggest that the surface structure remains Pt3Co, although the core changes from Pt to Pt3Co and to PtCo. At low Co loading, the bimetallic nanoparticles form a Pt3Co intermetallic surface alloy with Pt-rich core. With increasing Co loading, a full alloy forms where both the surface and NP compositions are Pt3Co. A further increase in Co loading leads to a Co-rich NP core, likely PtCo, with a surface of Pt3Co. Although Pt-Co intermetallic alloys form two different phases and several morphologies, the surface structures are similar in all catalysts. Although both monometallic Pt and Co are active for alkane dehydrogenation, all bimetallic Pt-Co catalysts are significantly more olefin selective than either single metal. The turnover rates of the bimetallic catalysts indicate that Pt is the active atom with little contribution from Co atoms. The high olefin selectivity is suggested to be due to Co acting as a less active structural promoter to break up large Pt ensembles in bimetallic NPs.},
doi = {10.1021/acscatal.9b00549},
journal = {ACS Catalysis},
number = 6,
volume = 9,
place = {United States},
year = {2019},
month = {4}
}

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Works referencing / citing this record:

Effect of Reduction of Pt–Sn/α-Al2O3 on Catalytic Dehydrogenation of Mixed-Paraffin Feed
journal, January 2020

  • Avithi Kanniappan, Suresh; Ragula, Udaya Bhaskar Reddy
  • Catalysts, Vol. 10, Issue 1
  • DOI: 10.3390/catal10010113