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Redox dynamics of Ni catalysts in CO2 reforming of methane

Paper ID Volume ID Publish Year Pages File Format Full-Text
53824 46986 2015 10 PDF Available
Title
Redox dynamics of Ni catalysts in CO2 reforming of methane
Abstract

•A Ni/Mg,Al-oxide catalyst was subjected to repeated TPR/O cylces.•The cycled Ni/MgAl2O4 -type catalyst exhibited lower Ni-oxide interaction.•The fresh and the cycled catalysts performed stably in dry reforming of methane.•The cycled catalyst showed a significantly lower degree of coke formation at 900 °C.•Redox pre-treatment can help mitigating the coking of Ni catalysts.

The influence of redox dynamics of a Ni/MgAl oxide catalyst for dry reforming of methane (DRM) at high temperature was studied to correlate structural stability with catalytic activity and coking propensity. Structural aging of the catalyst was simulated by repeated temperature-programmed reduction/oxidation (TPR/TPO) cycles. Despite a very high Ni loading of 55.4 wt.%, small Ni nanoparticles of 11 nm were obtained from a hydrotalcite-like precursor with a homogeneous distribution. Redox cycling gradually changed the interaction of the active Ni phase with the oxide support resulting in a crystalline Ni/MgAl2O4-type catalyst. After cycling the average particle size increased from 11 to 21 nm – while still a large fraction of small particles was present – bringing about a decrease in Ni surface area of 72%. Interestingly, the redox dynamics and its strong structural and chemical consequences were found to have only a moderate influence on the activity in DRM at 900 °C, but lead to a stable attenuation of carbon formation due to a lower fraction of graphitic carbon after DRM in a fixed-bed reactor. Supplementary DRM experiments in a thermobalance revealed that coke formation as a continuous process until a carbon limit is reached and confirmed a higher coking rate for the cycled catalyst.

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Keywords
Dry reforming of methane; Nickel; Coking; Ni, Mg, Al hydrotalcite; High temperature; Redox dynamics
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Publisher
Database: Elsevier - ScienceDirect
Journal: Catalysis Today - Volume 242, Part A, 15 March 2015, Pages 101–110
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
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