Journal
CHEMCATCHEM
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202201449
Keywords
alkali metals; Co3O4; density functional theory; N2O decomposition; oxygen vacancies
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In this study, the effect of alkali metal deposition on the activity of x-Co3O4 catalysts for the N2O catalytic decomposition was investigated. The results showed that the deposition of alkali metal Na improved the activity of the Na-Co3O4 catalyst, while the deposition of other alkali metals suppressed the catalytic decomposition of N2O. Characterization analysis indicated that the deposition of alkali metals did not change the morphology and structure of the catalysts but affected the chemical environment around the Co ion.
In this paper, the effect of alkali metal deposition on the activity of x-Co3O4 (x=Na, K, Rb, Cs) catalysts for the N2O catalytic decomposition was systematically explored by DFT calculation and various experimental characterization methods. The results demonstrated that the deposition of alkali metal Na improved the activity of the Na-Co3O4 catalyst for N2O catalytic decomposition at low temperatures. By contrast, the deposition of other alkali metals (K, Rb and Cs) suppressed the catalytic decomposition of N2O perceptibly. Analysis of the results of XRD, FT-IR, SEM, TEM, XPS, O-2-TPD and H-2-TPR characterization of x-Co3O4 catalysts showed that the deposition of alkali metals did not affect the morphology and structure of the catalysts. However, it affected the chemical environment around the Co ion in the x-Co3O4 catalyst, where the deposition of alkali metal Na not only facilitated the reduction of Co3+ to Co2+, but also promoted the surface decomposition step of N2O (i. e., the oxidation of Co2+ to Co3+ by giving electrons) at low temperatures, indicating that alkali metal Na improved the electron donating capability of the catalyst active center and enhanced the performance of the Na-Co3O4 catalyst for the DCD of N2O at low temperatures. The deposition of other alkali metals did not show the same results as that of alkali metal Na, indicating that the promotion of different alkali metals was different and would directly affect the catalytic effect. At low temperatures, the catalytic activity of catalysts deposited with the alkali metal Na was greater than that of catalysts deposited with other alkali metals.
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