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Title: Differences in the Nature of Active Sites for Methane Dry Reforming and Methane Steam Reforming over Nickel Aluminate Catalysts

Abstract

In this paper, the Pechini synthesis was used to prepare nickel aluminate catalysts with the compositions NiAl 4O 7, NiAl 2O 4, and Ni 2Al 2O 5. The samples have been characterized by N 2 physisorption, temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and X-ray absorption spectroscopy (XAS). Characterization results indicate unique structural properties and excellent regeneration potential of nickel aluminates. Prepared samples were tested when unreduced and reduced prior to reaction for methane dry reforming and methane steam reforming reactivity. NiAl 2O 4 in the reduced and unreduced state as well as NiAl 4O 7 in the reduced state are active and stable for methane dry reforming due to the presence of 4-fold coordinated oxidized nickel. The limited amount of metallic nickel in these samples minimizes carbon deposition. Finally, on the other hand, the presence of metallic nickel is required for methane steam reforming. Ni 2Al 2O 5 in the reduced and unreduced states and NiAl 2O 4 in the reduced state are found to be active for methane steam reforming due to the presence of sufficiently small nickel nanoparticles that catalyze the reaction without accumulating carbonaceous deposits.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [5]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering. Renewable Bioproducts Inst.; The Dow Chemical Company, Freeport, TX (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
  3. Micromeritics Instrument Corporation, Norcross, GA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Technology Division
  5. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering. Renewable Bioproducts Inst.
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Technology Division; Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Georgia Inst. of Technology, Atlanta, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); The Dow Chemical Company (United States); Georgia Institute of Technology (United States)
Contributing Org.:
Micromeritics Instrument Corporation, Norcross, GA (United States); The Dow Chemical Company, Freeport, TX (United States); Purdue Univ., West Lafayette, IN (United States)
OSTI Identifier:
1341645
Report Number(s):
BNL-113364-2016-JA
Journal ID: ISSN 2155-5435; TRN: US1701775
Grant/Contract Number:  
AC02-06CH11357; AC02-98CH10886
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 9; 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; Spinel; Synthesis gas; X-ray absorption spectroscopy; Coordination number; Regeneration

Citation Formats

Rogers, Jessica L., Mangarella, Michael C., D’Amico, Andrew D., Gallagher, James R., Dutzer, Michael R., Stavitski, Eli, Miller, Jeffrey T., and Sievers, Carsten. Differences in the Nature of Active Sites for Methane Dry Reforming and Methane Steam Reforming over Nickel Aluminate Catalysts. United States: N. p., 2016. Web. doi:10.1021/acscatal.6b01133.
Rogers, Jessica L., Mangarella, Michael C., D’Amico, Andrew D., Gallagher, James R., Dutzer, Michael R., Stavitski, Eli, Miller, Jeffrey T., & Sievers, Carsten. Differences in the Nature of Active Sites for Methane Dry Reforming and Methane Steam Reforming over Nickel Aluminate Catalysts. United States. doi:10.1021/acscatal.6b01133.
Rogers, Jessica L., Mangarella, Michael C., D’Amico, Andrew D., Gallagher, James R., Dutzer, Michael R., Stavitski, Eli, Miller, Jeffrey T., and Sievers, Carsten. Wed . "Differences in the Nature of Active Sites for Methane Dry Reforming and Methane Steam Reforming over Nickel Aluminate Catalysts". United States. doi:10.1021/acscatal.6b01133. https://www.osti.gov/servlets/purl/1341645.
@article{osti_1341645,
title = {Differences in the Nature of Active Sites for Methane Dry Reforming and Methane Steam Reforming over Nickel Aluminate Catalysts},
author = {Rogers, Jessica L. and Mangarella, Michael C. and D’Amico, Andrew D. and Gallagher, James R. and Dutzer, Michael R. and Stavitski, Eli and Miller, Jeffrey T. and Sievers, Carsten},
abstractNote = {In this paper, the Pechini synthesis was used to prepare nickel aluminate catalysts with the compositions NiAl4O7, NiAl2O4, and Ni2Al2O5. The samples have been characterized by N2 physisorption, temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and X-ray absorption spectroscopy (XAS). Characterization results indicate unique structural properties and excellent regeneration potential of nickel aluminates. Prepared samples were tested when unreduced and reduced prior to reaction for methane dry reforming and methane steam reforming reactivity. NiAl2O4 in the reduced and unreduced state as well as NiAl4O7 in the reduced state are active and stable for methane dry reforming due to the presence of 4-fold coordinated oxidized nickel. The limited amount of metallic nickel in these samples minimizes carbon deposition. Finally, on the other hand, the presence of metallic nickel is required for methane steam reforming. Ni2Al2O5 in the reduced and unreduced states and NiAl2O4 in the reduced state are found to be active for methane steam reforming due to the presence of sufficiently small nickel nanoparticles that catalyze the reaction without accumulating carbonaceous deposits.},
doi = {10.1021/acscatal.6b01133},
journal = {ACS Catalysis},
number = 9,
volume = 6,
place = {United States},
year = {Wed Jul 20 00:00:00 EDT 2016},
month = {Wed Jul 20 00:00:00 EDT 2016}
}

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