4.8 Article

Designing perovskite catalysts for controlled active-site exsolution in the microwave dry reforming of methane

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 284, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2020.119711

Keywords

Dry reforming of methane; Microwave; In situ XRD; Perovskite; Lanthanum strontium cobaltite

Funding

  1. US Department of Energy's Fossil Energy Crosscutting Technology Research Program
  2. RSS [89243318CFE000003]
  3. DOE Office of Science [DE-SC0012704, DE-AC02 06CH11357]

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The dry reforming of methane (DRM) is a promising process for generating syngas while consuming CO2, but industrial applications have been limited due to the high temperatures required to prevent coke formation. Microwave-assisted DRM (MW-DRM) is a promising approach that can utilize excess renewable electrons to rapidly and selectively heat the catalyst bed. Catalyst doping studies have shown that the addition of oxophilic transition metals prevents over-reduction and stabilizes the perovskitic phases under reaction conditions.
The dry reforming of methane (DRM) is a promising process for generating syngas (CO + H-2) while consuming CO2, but industrial applications have been limited due to the high temperatures required to prevent coke formation. Microwave-assisted DRM (MW-DRM) is a promising approach to enable high temperature reactions because it can utilize excess renewable electrons to rapidly and selectively heat the catalyst bed without wasting time and energy heating the entire reactor. Here we demonstrate the MW-DRM reaction by modifying lanthanum strontium cobaltite (LSC) to serve as both microwave absorber and catalyst. Catalyst doping studies revealed the addition of oxophilic transition metals prevented over-reduction and stabilized the perovskitic phases under reaction conditions. In situ, synchrotron-based x-ray diffraction revealed the catalyst becomes active once metallic cobalt forms on a retained perovskitic support. The best performing Mn doped LSC catalyst showed 80-90 % single-pass conversions, stable operation for over 10 h, and easy microwave regeneration.

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