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

Rogers, Jessica L.; Mangarella, Michael C.; D’Amico, Andrew D.; Gallagher, James R.; Dutzer, Michael R.; Stavitski, Eli; Miller, Jeffrey T.; Sievers, Carsten

doi:10.1021/acscatal.6b01133

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

Journal Article · Wed Jul 20 00:00:00 EDT 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b01133· OSTI ID:1341645

Rogers, Jessica L. ^[1]; Mangarella, Michael C. ^[2]; D’Amico, Andrew D. ^[3]; Gallagher, James R. ^[4]; Dutzer, Michael R. ^[5]; Stavitski, Eli ^[6]; Miller, Jeffrey T. ^[7]; Sievers, Carsten ^[5]

Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering. Renewable Bioproducts Inst.; The Dow Chemical Company, Freeport, TX (United States)
Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
Micromeritics Instrument Corporation, Norcross, GA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Technology Division
Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering. Renewable Bioproducts Inst.
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Technology Division; Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); Georgia Institute of Technology, Atlanta, GA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); The Dow Chemical Company (United States); Georgia Institute of Technology (United States)

Contributing Organization:: Micromeritics Instrument Corporation, Norcross, GA (United States); The Dow Chemical Company, Freeport, TX (United States); Purdue Univ., West Lafayette, IN (United States)

Grant/Contract Number:: AC02-06CH11357; AC02-98CH10886

OSTI ID:: 1341645

Report Number(s):: BNL-113364-2016-JA; TRN: US1701775

Journal Information:: ACS Catalysis, Vol. 6, Issue 9; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 128 works

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