4.7 Article

Gd-Ru Nanoparticles Supported on Zr0.5Ce0.5O2 Nanorods for Dry Methane Reforming

期刊

ACS APPLIED NANO MATERIALS
卷 4, 期 3, 页码 2547-2557

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.0c03140

关键词

Ru/Zr0.5Ce0.5O2; Gd2O3 promotion; dry reforming of methane; hydrothermal synthesis; activation energy

资金

  1. Council of Scientific and Industrial Research, India [MLP 1089]

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This study investigated the utilization of a robust Ru-based catalyst prepared through hydrothermal synthesis for dry reforming of methane. The addition of an optimal amount of Gd2O3 promoted catalyst stability by leading to smaller Ru particle size and inhibiting coke deposition. Additionally, the promotion with 0.5% Gd2O3 lowered the apparent activation energy of methane conversion and showed preference for methane cracking over Ru atoms and CO2 activation on Gd atoms.
Dry reforming of methane is considered a potential reaction for the utilization of waste greenhouse gases to generate valuable chemicals. However, catalyst deactivation under a harsh reaction condition appears as the main obstacle toward its commercialization. In the present work, a facile hydrothermal synthesis procedure was adopted to prepare a robust Ru-based catalyst. Among the various combinations, a 1% Ru supported over Zr0.5Ce0.5O2 nanorod catalyst showed enhanced coke resistance and almost stable activity during 200 h activity analysis. Promotion of Ru/Zr0.5Ce0.5O2 with an optimum amount of Gd2O3 improved catalyst stability, which was attributed to the strong interaction of Ru with Gd2O3 leading to smaller Ru particle size (similar to 5 nm) and an improved OSC was inhibiting coke deposition. Promotion with 0.5% Gd2O3 further lowered the apparent activation energy of methane conversion to similar to 20.6 kcal/mol without changing the reaction orders significantly. DFT calculation confirmed, due to the orbital similarity, methane cracking is preferred over Ru atoms and CO2 activation occurred on Gd atoms.

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