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Co₃ O₄ -CeO₂ Nanocomposites for Low-Temperature CO Oxidation.

ABSTRACT: In an effort to combine the favorable catalytic properties of Co₃ O₄ and CeO₂ , nanocomposites with different phase distribution and Co₃ O₄ loading were prepared and employed for CO oxidation. Synthesizing Co₃ O₄ -modified CeO₂ via three different sol-gel based routes, each with 10.4 wt % Co₃ O₄ loading, yielded three different nanocomposite morphologies: CeO₂ -supported Co₃ O₄ layers, intermixed oxides, and homogeneously dispersed Co. The reactivity of the resulting surface oxygen species towards CO were examined by temperature programmed reduction (CO-TPR) and flow reactor kinetic tests. The first morphology exhibited the best performance due to its active Co₃ O₄ surface layer, reducing the light-off temperature of CeO₂ by about 200 °C. In contrast, intermixed oxides and Co-doped CeO₂ suffered from lower dispersion and organic residues, respectively. The performance of Co₃ O₄ -CeO₂ nanocomposites was optimized by varying the Co₃ O₄ loading, characterized by X-ray diffraction (XRD) and N₂ sorption (BET). The 16-65 wt % Co₃ O₄ -CeO₂ catalysts approached the conversion of 1 wt % Pt/CeO₂ , rendering them interesting candidates for low-temperature CO oxidation.

SUBMITTER: Yang J

PROVIDER: S-EPMC9292333 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:CO elimination through oxidation over highly active and cost-effective catalysts is a way forward for many processes of industrial and environmental importance. In this study, doped CeO2 with transition metals (TM = Cu, Co, Mn, Fe, Ni, Zr, and Zn) at a level of 20 at. % was tested for CO oxidation. The oxides were prepared using microwave-assisted sol-gel synthesis to improve catalyst's performance for the reaction of interest. The effect of heteroatoms on the physicochemical properties (structure, morphology, porosity, and reducibility) of the binary oxides M-Ce-O was meticulously investigated and correlated to their CO oxidation activity. It was found that the catalytic activity (per gram basis or TOF, s-1) follows the order Cu-Ce-O > Ce-Co-O > Ni-Ce-O > Mn-Ce-O > Fe-Ce-O > Ce-Zn-O > CeO2. Participation of mobile lattice oxygen species in the CO/O2 reaction does occur, the extent of which is heteroatom-dependent. For that, state-of-the-art transient isotopic 18O-labeled experiments involving 16O/18O exchange followed by step-gas CO/Ar or CO/O2/Ar switches were used to quantify the contribution of lattice oxygen to the reaction. SSITKA-DRIFTS studies probed the formation of carbonates while validating the Mars-van Krevelen (MvK) mechanism. Scanning transmission electron microscopy-high-angle annular dark field imaging coupled with energy-dispersive spectroscopy proved that the elemental composition of dopants in the individual nanoparticle of ceria is less than their composition at a larger scale, allowing the assessment of the doping efficacy. Despite the similar structural features of the catalysts, a clear difference in the Olattice mobility was also found as well as its participation (as expressed with the α descriptor) in the reaction, following the order αCu > αCo> αMn > αZn. Kinetic studies showed that it is rather the pre-exponential (entropic) factor and not the lowering of activation energy that justifies the order of activity of the solids. DFT calculations showed that the adsorption of CO on the Cu-doped CeO2 surface is more favorable (-16.63 eV), followed by Co, Mn, Zn (-14.46, -4.90, and -4.24 eV, respectively), and pure CeO2 (-0.63 eV). Also, copper compensates almost three times more charge (0.37e-) compared to Co and Mn, ca. 0.13e- and 0.10e-, respectively, corroborating for its tendency to be reduced. Surface analysis (X-ray photoelectron spectroscopy), apart from the oxidation state of the elements, revealed a heteroatom-ceria surface interaction (Oa species) of different extents and of different populations of Oa species.

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Co₃ O₄ -CeO₂ Nanocomposites for Low-Temperature CO Oxidation.

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