4.8 Article

Spherical Ni Nanoparticles Supported by Nanosheet-Assembled Al2O3 for Dry Reforming of CH4: Elucidating the Induction Period and Its Excellent Resistance to Coking

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 49, Pages 58605-58618

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c17890

Keywords

spherical Ni nanoparticles; nanosheet-assembled Al2O3; dry reforming of methane; induction period; resistance to coking

Funding

  1. National Key Research and Development Program of China [2016YFC0204300]
  2. National Natural Science Foundation of China [21808142]
  3. Fundamental Research Funds for the Central Universities

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Using nanosheet-assembled Al2O3 as support for Ni nanoparticles, the catalyst shows superior long-term stability and coking resistance in the dry reforming of methane reaction. The active Ni species are aggregated into Ni nanoparticles, stabilized by the hierarchical hollow microspheres of the support. The catalyst's excellent performance is attributed to the formation of spherical Ni nanoparticles, superior CO2 adsorption ability, and more surface hydroxyl groups on the support.
The design and preparation of efficient coking-resistant catalysts for dry reforming of methane (DRM) is significant for industrial applications but a challenge for supported Ni catalysts. Nanosheet-assembled Al2O3 (NA-Al2O3) with hierarchical hollow microspheres was used to support Ni nanoparticles, which exhibits superior long-time stability and coking resistance for the DRM reaction from 700 to 800 degrees C without coke deposition. Active Ni species, exsolved from NiAl2O4 spinel, are aggregated into Ni nanoparticles and finally stabilize as spherical Ni nanoparticles of 18.0 nm due to the spatial confinement of hierarchical hollow microspheres of the NA-Al2O3 support after the DRM reaction for 60 h. The catalytic activity in the induction period of the Ni/(NA-Al2O3) catalyst increases because of the enhancement of the surface Ni-0/(Ni-0+Ni2+) ratio, that is, the increment of the amount of active Ni sites. The spherical Ni nanoparticles embedded in the NA-Al2O3 support, superior CO2 adsorption ability, and more surface hydroxyl groups on the Ni/(NA-Al2O3) catalyst are the determining factors for its long-time stability and excellent anti-coking for the DRM reaction.

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