期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 13, 期 10, 页码 3035-3046出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d3cy00253e
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In this study, porous CeO2/OLC was prepared as a support and nanoreactor for PdNiO, and it exhibited high activity for electrochemical CO oxidation due to the electronic interaction between PdNiO and CeO2/OLC support.
Porous ternary Pd-based catalysts are highly promising for various electrocatalytic applications, due to their low Pd mass, high surface area, accessible active sites, and tunable electronic structure; however, their activity for CO oxidation (COoxid) in different electrolytes is yet to be reported. Herein, ternary PdNiO nanocrystals supported on porous CeO2/onion-like carbon nanostructures (PdNiO-CeO2/OLC) were prepared by the sol-gel and impregnation approaches for electrochemical COoxid in different electrolytes at room temperature. Notably, porous CeO2/OLC acts as a support and nanoreactor for supporting the growth of PdNiO without the need for reducing agents or surfactants. The as-obtained PdNiO-CeO2/OLC had a porous sponge-like structure composed of ultra-small PdNiO nanocrystals (8 +/- 1 nm) distributed on porous flower-like CeO2 and OLC, which possessed unique merits of multifunctional structure, clean surface, low mass of Pd (10 wt%), porosity (0.30 cm(3) g(-1)), and high surface area (155.66 m(2) g(-1)). The COoxid activity of PdNiO-CeO2/OLC was higher than those of PdNiO/OLC, PdNiO-CeO2, and commercial Pd/C catalyst, owing to the electronic interaction of PdNiO with CeO2/OLC support, which eases CO adsorption/activation alongside activation/dissociation of H2O to generate active oxygenated species (i.e., OH) needed for accelerating COoxid kinetics. The COoxid activity of PdNiO-CeO2/OLC in acidic electrolyte (HClO4) was better than those in alkaline (KOH) and neutral (NaHCO3) electrolytes. This study may open new doorways for understanding the effect of electrolytes and supports on the COoxid activity of porous ternary Pd-based catalysts.
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