Three-dimensionally ordered macroporous Co3O4 (3DOM Co3O4) and its supported gold (xAu/3DOM Co3O4, x = 1.1-8.4 wt%) nanocatalysts were prepared using the polymethyl methacrylate-templating and bubble-assisted polyvinyl alcohol-protected reduction methods, respectively. The 3DOM Co3O4 and xAu/3DOM Co3O4 samples exhibited a surface area of 22-27 m(2) g(-1). The Au nanoparticles with a size of 2.4-3.7 nm were uniformly deposited on the macropore walls of 3DOM Co3O4. There were good correlations of oxygen adspecies concentration and low-temperature reducibility with catalytic activity of the sample for CO and toluene oxidation. Among 3DOM Co3O4 and xAu/3DOM Co3O4, the 6.5Au/3DOM Co3O4 sample performed the best, giving a T90% (the temperature required for achieving a conversion of 90%) of -35 °C at a space velocity of 20 000 mL g(-1) h(-1) for CO oxidation and 256 °C at a space velocity of 40 000 mL g(-1) h(-1) for toluene oxidation. The effect of water vapor was more significant in toluene oxidation than in CO oxidation. The apparent activation energies (26 and 74 kJ mol(-1)) over 6.5Au/3DOM Co3O4 were lower than those (34 and 113 kJ mol(-1)) over 3DOM Co3O4 for CO and toluene oxidation, respectively. It is concluded that the higher oxygen adspecies concentration, better low-temperature reducibility, and strong interaction between Au and 3DOM Co3O4 were responsible for the excellent catalytic performance of 6.5Au/3DOM Co3O4.
Uniform hollow spherical rhombohedral LaMO3 and solid spherical cubic MOx (M = Mn and Co) NPs were fabricated using the PMMA-templating strategy. Hollow spherical LaMO3 and solid spherical MOx NPs possessed surface areas of 21-33 and 21-24 m(2)/g, respectively. There were larger amounts of surface-adsorbed oxygen species and better low-temperature reducibility on/of the hollow spherical LaMO3 samples than on/of the solid spherical MOx samples. Hollow spherical LaMO3 and solid spherical MOx samples outperformed their nanosized counterparts for oxidation of CO and toluene, with the best catalytic activity being achieved over the solid spherical Co3O4 sample for CO oxidation (T50% = 81 °C and T90% = 109 °C) at space velocity = 10,000 mL/(g h) and the hollow spherical LaCoO3 sample for toluene oxidation (T50% = 220 °C and T90% = 237 °C) at space velocity = 20,000 mL/(g h). It is concluded that the higher surface areas and oxygen adspecies concentrations and better low-temperature reducibility are responsible for the excellent catalytic performance of the hollow spherical LaCoO3 and solid spherical Co3O4 NPs. We believe that the PMMA-templating strategy provides an effective route to prepare uniform perovskite-type oxide and transition-metal oxide NPs.
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