Abstract

In this study, we report the formation of needle-shaped NiAl2O4 via favorable interactions between Ni and Al species over macroporous Ni/CexZr1-xO2–Al2O3 catalysts for dry reforming of methane (DRM) and its remarkable improvement in the catalytic performance. The macroporous catalysts prepared by a one-pot (OP) method promote a favorable interaction between Ni and Al species that results in the formation of unique needle-shaped NiAl2O4 due to easy access to each other compared with that by incipient wetness impregnation. The NiAl2O4 phase in the calcined catalysts transforms into highly dispersed Ni and defective Al2O3 via the Ni exsolution in the reduction step. The presence of oxygen vacancies near Ni0 species facilitates the CO2 activation and enhances the catalyst stability over DRM. The optimized distribution of active sites with abundant defects over macroporous Ni/CexZr1-xO2-Al2O3 catalysts (OP) result in high conversions of CH4 and CO2 and a low coking rate in DRM.

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