Catalytically stable monodispersed multi-core Ni-Co nanoparticles encapsulated with SiO2 shells for dry reforming of CH4 with CO2

Journal of CO2 Utilization(2022)

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摘要
Enhanced thermal and catalytic stability of monodispersed Ni-Co bimetal nanoparticles with its even size distribution of ~6 nm encapsulated by SiO2 shell (NC@Si) having multicore-shell structures were verified for a harsh dry reforming of methane with CO2 (DRM). The extents of coke formations and aggregations of Ni-Co nanoparticles were dramatically suppressed with positive contributions of oxophilic Co species as well as by their spatial confinement effects. The optimal N8C2@Si with a Ni/Co molar ratio of ~4 revealed a relatively higher CH4 and CO2 conversion of 74.1% and 83.7% at T = 800 °C without significant deactivation phenomena. The original morphologies of the monodispersed Ni-Co nanoparticles were well preserved even after a long-run DRM reaction for 120 h with an insignificant coke formation and active metal aggregation. The superior catalytic activity and stability of the N8C2@Si and N9C1@Si were attributed to the highly-dispersed oxophilic metallic cobalt oxides in the monodispersed stable Ni-Co nanoparticles, which enhanced CO2 adsorption capacity as well as increased thermal stability of the spatially confined Ni-Co nanoparticles with the help of mesoporous SiO2 shell at its optimal aging time less than 4 h. The new multicore-shell structures of the N8C2@Si can effectively suppress the filamentous coke formations as well as minimize the Ni-Co multicore aggregations by stronger metal-SiO2 interactions in the mesoporous protective SiO2 shells.
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关键词
Multicore-shell structured Ni-Co@SiO2,Dry reforming of methane with CO2 (DRM),Ni-Co nanoparticles,Spatial confinement effects,Deactivation by coke precursors
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