Influence of the Surface Species over Co3O4 on the Formaldehyde Catalytic Oxidation Performance†

doi:10.7503/cjcu20140757

Abstract

Abstract:

The Co₃O₄ catalysts were prepared via precipitation methods, and then were pretreated in N₂ or O₂ at different temperatures. Based on the study of formaldehyde catalytic oxidation, the catalytic performances were investigated with the detailed surface characterization via temperature programmed desorption(O₂/CO₂-TPD, HCHO-TPSR), thermogravimetric-differential scanning calorimetry(TG-DSC) and in situ diffuse reflectance infrared fourier transform spectroscopy(in situ DRIFTS). The results presented that Co₃O₄-N₂-200 showed the optimal catalytic performance, because there were rich unsaturated coordination centers of Co³⁺ and negative oxygen ions with weak bond strength on the surface of Co₃O₄-N₂-200, which was ready to adsorb formaldehyde to form bidentate formate, and then decompose to products via monodentate formate. With increasing pretreatment temperature, the amount of negative oxygen ions decreased, accordingly the catalytic activity for formaldehyde catalytic oxidation decreased due to slow decomposition rate of desorbed bidentate formate.

Key words: Formaldehyde catalytic oxidation, Co₃O₄, Formate, Temperature programmed desorption, In situ diffuse reflectance infrared Fourier transform spectroscopy, Surface oxygen species

CLC Number:

O646

TrendMD:

ZHANG Ye, ZHOU Jiajia, WU Guisheng, MAO Dongsen, LU Guanzhong. Influence of the Surface Species over Co₃O₄ on the Formaldehyde Catalytic Oxidation Performance^†[J]. Chem. J. Chinese Universities, 2014, 35(12): 2598.

Figures/Tables 8

Fig.1 Catalytic activity(A) and CO2 selectivity(B) of Co3O4 pretreated in N2 or O2 at different temperatures a. Room temperature; b. N2, 200 ℃; c. N2, 300 ℃; d. N2, 400 ℃; e. O2, 200 ℃; f. O2, 400 ℃.

Fig.2 Dependency of formaldehyde conversion(A) and CO2 selectivity(B) on the reaction time over Co3O4-N2-200(a) and Co3O4-N2-400(b) at 100 ℃

Fig.3 XRD pattern(A) of Co3O4 as prepared and IR spectra(B) of Co3O4 pretreated in N2 at 200 ℃(a), 300 ℃(b) and 400 ℃(c)

Fig.4 TG-DSC curve of Co3O4 catalyst in N2(50 mL/min) at a rate of 5 ℃/min

Fig.5 O2-TPD(A) and CO2-TPD(B) profiles over Co3O4 catalysts pretreated in N2 at 200 ℃(a), 300 ℃(b) and 400 ℃(c)

Fig.6 FTIR spectra of adsorbed formaldehyde over Co3O4-N2-25(a), Co3O4-N2-200(b) and Co3O4-N2-400(c) for 20 min

Fig.7 HCHO-TPSR profiles over Co3O4-N2-200(A) and Co3O4-N2-400(B)

Scheme 1 Reaction mechanism diagram of formaldehyde oxidation over Co3O4

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Influence of the Surface Species over Co₃O₄ on the Formaldehyde Catalytic Oxidation Performance^†

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