4.7 Article

Roles of metal oxide overlayers on hydrotalcite-structured Ni-MgAlOx for dry reforming of CH4 with CO2

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FUEL PROCESSING TECHNOLOGY
卷 250, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.fuproc.2023.107895

关键词

Dry reforming of methane (DRM); Confined Ni nanoparticles; Overlayer coating method; Hydrotalcite-like Ni-MgAl 2 O 4; Exsolution process; Oxygen vacant sites

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By introducing a coating layer of four different metal oxides (CeO2, ZrO2, SiO2, and Al2O3) on the coprecipitated hydrotalcite-like Ni-MgAl2O4 (NiMgAl), the thermal stability of Ni nanoparticles in the dry reforming reaction of CH4 with CO2 (DRM) was enhanced. Among the catalysts, NiMgAl@Al showed superior catalytic properties due to the stronger metal support interaction (SMSI) resulting from the spatially confined Ni nanoparticles on the MgAl2O4 frameworks through exsolution phenomena facilitated by the porous Al2O3 overlayers. The simpler overlayer coating method, especially with porous Al2O3 coating layer, was found to be an effective way to achieve superior catalytic activity and stability by preserving thermally stable smaller Ni nanoparticles on the Ni-MgAl2O4 surfaces.
The thermal stability of Ni nanoparticles on the coprecipitated hydrotalcite-like Ni-MgAl2O4 (NiMgAl) was enhanced by simply introducing an overlayer coating method with four different metal oxides (M) such as CeO2, ZrO2, SiO2 and Al2O3 (NiMgAl@M) for a harsh dry reforming reaction of CH4 with CO2 (DRM). Among the catalysts, the superior catalytic properties on the NiMgAl@Al such as less sintering and coke deposition were originated from the much stronger metal support interaction (SMSI), which were originated from the formed spatially confined Ni nanoparticles on the MgAl2O4 frameworks through the possible exsolution phenomena with the help of the porous Al2O3 overlayers. The unmodified NiMgAl catalyst revealed a relatively lower catalytic activity due to the facile coke depositions, which was mainly caused by the selective formation of larger Ni nanoparticles above 25 nm with its heterogeneous size distribution. The much simpler overlayer coating method with the porous overlayer structures, especially for Al2O3 coating layer, was found to be an effective way to achieve a superior catalytic activity and stability by preserving the thermally stable smaller Ni nanoparticles on the hydrotalcite-like Ni-MgAl2O4 surfaces.

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