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Published on: December 6, 2021
Ligand-Mediated Cobalt Oxide Nanocatalysts Unlocking Efficient Toluene Oxidation: Facet Engineering and Morphology
Mingyang Ma1, Ruhan Zhang1, Yanan Shen1
1School of Environment and Materials Engineering, Yantai University, Yantai 264005, P. R. China.
Abstract:
Regulating the oxygen vacancy concentration and active sites of Co3O4 through crystal facet engineering and morphological modulation can significantly optimize its catalytic performance. In this study, a ligand-mediated synergistic strategy for crystal facet and morphology regulation was employed to construct Co3O4 catalysts exposing distinct facets, including {001}, {011}, {111}, and {110}, and the catalytic activity of these catalysts was evaluated for the oxidation of toluene. Catalytic tests revealed that Co3O4-S achieved a T90 (temperature for 90% toluene conversion) of 259 °C, with the activity order being dodecahedron Co3O4-S {110} > flower-like Co3O4-H {011} > disciform Co3O4-Y {111} > cube-type Co3O4-L {001}. The superior catalytic activity of Co3O4-S is attributed to its exposed {110} crystal facets, which feature abundant oxygen vacancies, a higher concentration of Co3+ active sites, and a larger specific surface area. Density functional theory (DFT) calculations reveal that the {110} crystal plane of Co3O4-S features the lowest oxygen vacancy formation energy (EVO {110} = 4.41 eV), the optimal O2 adsorption energy (Eads {110} = -1.88 eV), and toluene adsorption energy (Eads {110} = -2.38 eV), indicating strong ability for oxygen activation. This study clarifies the mechanism of the ligand-mediated facet-morphology synergistic regulation strategy, establishes a complete structure-activity chain of "facet/morphology → oxygen vacancy → adsorption energy → catalytic activity" for toluene oxidation, and provides key theoretical support and technical references for the rational design of high-efficiency non-noble metal catalysts for toluene oxidation.
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