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Title: Exsolution of Re-alloy catalysts with enhanced stability for methane dry reforming

Authors:
; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
FOREIGN
OSTI Identifier:
1349935
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Catalysis. B, Environmental; Journal Volume: 209
Country of Publication:
United States
Language:
ENGLISH

Citation Formats

Zubenko, Daria, Singh, Sarika, and Rosen, Brian A. Exsolution of Re-alloy catalysts with enhanced stability for methane dry reforming. United States: N. p., 2017. Web. doi:10.1016/j.apcatb.2017.03.047.
Zubenko, Daria, Singh, Sarika, & Rosen, Brian A. Exsolution of Re-alloy catalysts with enhanced stability for methane dry reforming. United States. doi:10.1016/j.apcatb.2017.03.047.
Zubenko, Daria, Singh, Sarika, and Rosen, Brian A. Sat . "Exsolution of Re-alloy catalysts with enhanced stability for methane dry reforming". United States. doi:10.1016/j.apcatb.2017.03.047.
@article{osti_1349935,
title = {Exsolution of Re-alloy catalysts with enhanced stability for methane dry reforming},
author = {Zubenko, Daria and Singh, Sarika and Rosen, Brian A.},
abstractNote = {},
doi = {10.1016/j.apcatb.2017.03.047},
journal = {Applied Catalysis. B, Environmental},
number = ,
volume = 209,
place = {United States},
year = {Sat Jul 01 00:00:00 EDT 2017},
month = {Sat Jul 01 00:00:00 EDT 2017}
}
  • Atomic layer deposition (ALD) was used to deposit Ni and Pt on alumina supports to form monometallic and bimetallic catalysts with initial particle sizes of 1–2.4 nm. The ALD catalysts were more active (per mass of metal) than catalysts prepared by incipient wetness (IW) for dry reforming of methane (DRM), and they did not form carbon whiskers during reaction due to their sufficiently small size. Catalysts modified by Pt ALD had higher rates of reaction per mass of metal and inhibited coking, whereas NiPt catalysts synthesized by IW still formed carbon whiskers. Temperature-programmed reduction of Ni catalysts modified by Ptmore » ALD indicated the presence of bimetallic interaction. Density functional theory calculations suggested that under reaction conditions, the NiPt surfaces form Ni-terminated surfaces that are associated with higher DRM rates (due to their C and O adsorption energies, as well as the CO formation and CH4 dissociation energies).« less
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  • 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 statemore » 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.« less
  • Partial oxidation and dry reforming of methane to synthesis gas over Ca/Ni/K(Na) catalysts have been studied. Effects of temperature, pressure, and oxygen/methane ratios on catalytic activity, selectivity, and carbon formation have been determined. Also reforming of 13CH4 in the presence of CO2 and Temperature-Programmed Oxidation (TPO) of deposited carbon after the reaction indicated that both methane and CO2 contribute to carbon formation. The TPO of deposited carbon on Ca/Ni/K catalyst showed that the catalyst consumed a significant amount of oxygen, only a fraction of which was consumed by carbon species on the surface, indicating that the surface oxygen plays amore » significant role in oxidizing and removing carbon species from the catalyst surfaces.« less