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Frontiers of Chemical Science and Engineering

Front. Chem. Sci. Eng.    2020, Vol. 14 Issue (6) : 937-947     https://doi.org/10.1007/s11705-019-1900-6
RESEARCH ARTICLE
Room temperature oxidation of acetone by ozone over alumina-supported manganese and cobalt mixed oxides
Mehraneh Ghavami1, Mostafa Aghbolaghy1, Jafar Soltan1(), Ning Chen1,2
1. Department of Chemical and Biological Engineering, University of Saskatchewan, Saskatoon, S7N 5A9, Canada
2. Canadian Light Source Inc., University of Saskatchewan, Saskatoon, S7N 0X4, Canada
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Abstract

Volatile organic compounds (VOCs) are among the major sources of air pollution. Catalytic ozonation is an efficient process for removing VOCs at lower reaction temperature compared to catalytic oxidation. In this study, a series of alumina supported single and mixed manganese and cobalt oxides catalysts were used for ozonation of acetone at room temperature. The influence of augmenting the single Mn and Co catalysts were investigated on the performance and structure of the catalyst. The manganese and cobalt single and mixed oxides catalysts of the formula Mn10%-CoX and Co10%-MnX (where X= 0, 2.5%, 5%, or 10%) were prepared. It was found that addition of Mn and Co at lower loading levels (2.5% or 5%) to single metal oxide catalysts enhanced the catalytic activity. The mixed oxides catalysts of (Mn10%-Co2.5%) and (Mn10%-Co5%) led to acetone conversion of about 84%. It is concluded that lower oxidation state of the secondary metal improves ozone decomposition and oxidation of acetone.

Keywords ozone      VOC      manganese oxides      cobalt oxides      alumina support     
Corresponding Author(s): Jafar Soltan   
Online First Date: 26 February 2020    Issue Date: 11 September 2020
 Cite this article:   
Mehraneh Ghavami,Mostafa Aghbolaghy,Jafar Soltan, et al. Room temperature oxidation of acetone by ozone over alumina-supported manganese and cobalt mixed oxides[J]. Front. Chem. Sci. Eng., 2020, 14(6): 937-947.
 URL:  
http://journal.hep.com.cn/fcse/EN/10.1007/s11705-019-1900-6
http://journal.hep.com.cn/fcse/EN/Y2020/V14/I6/937
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Mehraneh Ghavami
Mostafa Aghbolaghy
Jafar Soltan
Ning Chen
Fig.1  Schematic of the experimental setup.
Catalyst Mn and Co loading /wt-% SBET /(m2?g–1) Pore volume /(cm3?g−1)
Mn Co
g-Al2O3 220 0.61
Mn/g-Al2O3 10 200 0.56
Mn-Co/g-Al2O3 10 2.5 186 0.54
Mn-Co/g-Al2O3 10 5 178 0.53
Mn-Co/g-Al2O3 10 10 180 0.49
Co/g-Al2O3 10 210 0.59
Co-Mn/g-Al2O3 2.5 10 194 0.55
Co-Mn/g-Al2O3 5 10 183 0.52
Co-Mn/g-Al2O3 10 10 174 0.47
Tab.1  Chemical compositions and pore structures of the catalysts
Fig.2  XRD patterns of the alumina supported catalysts (Al2O3 *, Mn2O3 l, Mn3O4○, MnO2 +, Co3O4 n, CoO □).
Catalyst Mn2O3
particle size /nm
Mn
dispersion /%
Co3O4
particle size /nm
Co
dispersion /%
Mn10%/g-Al2O3 18 7
Mn10%-Co2.5%/g-Al2O3 26 5 Na) Na)
Mn10%-Co5%/g-Al2O3 20 7 13 5
Mn10%-Co10%/g-Al2O3 23 6 9 7
Co10%/g-Al2O3 14 4
Co10%-Mn2.5%/g-Al2O3 Na) Na) 21 3
Co10%-Mn5%/g-Al2O3 18 7 12 5
Co10%-Mn10%/g-Al2O3 18 7 12 5
Tab.2  Mn and Co oxides particle sizes and dispersions obtained from XRD spectra
Fig.3  Magnitude of the Fourier transform of EXAFS spectra: (a) Mn K-edge, (b) Co K-edge.
Catalyst Mn3O4 /% Mn2O3 /% MnO2 /% CoO /% Co3O4 /%
Mn10%/g-Al2O3 7 82 11
Mn10%-Co2.5%/g-Al2O3 20 80 0 45 55
Mn10%-Co5%/g-Al2O3 16 84 0 44 56
Mn10%-Co10%/g-Al2O3 7 85 8 16 84
Co10%/g-Al2O3 100
Co10%-Mn2.5%/g-Al2O3 69 29 2 100
Co10%-Mn5%/g-Al2O3 54 44 2 2 98
Co10%-Mn10%/g-Al2O3 27 73 0 3 97
Tab.3  Result of linear combination fitting of Mn and Co K-edge XANES
Fig.4  Acetone and ozone conversions (%) at 25°C and 150 min of reaction, [acetone] = 150 ppm, and [O3] = 1200 ppm, catalyst weight= 0.065 g, gas flow rate= 250 mL?min1.
Catalyst Acetone oxidation rate
/(×105 mol?min1?g-1)
Ozone decomposition rate
/(×105 mol?min1?g-1)
COx yield /%
Mn10%/g-Al2O3 1.57 11.26 91.31
Mn10%-Co2.5%/g-Al2O3 1.98 17.01 90.41
Mn10%-Co5%/g-Al2O3 1.98 17.34 90.53
Mn10%-Co10%/g-Al2O3 1.25 9.07 92.98
Co10%/g-Al2O3 1.15 8.00 95.71
Co10%-Mn2.5%/g-Al2O3 1.76 12.16 88.21
Co10%-Mn5%/g-Al2O3 1.35 7.60 91.48
Co10%-Mn10%/g-Al2O3 1.21 5.39 96.58
Tab.4  Catalytic activity of single and mixed metal oxides catalysts for acetone ozonation at 150 min of reaction a)
Fig.5  CO% and CO2% in the reaction product stream at 25°C and 150 min of reaction, [acetone] = 150 ppm, and [O3] = 1200 ppm, catalyst weight= 0.065 g, gas flow rate= 250 mL?min1.
Fig.6  Long-term activity and product formation of Mn10%-Co2.5%/γ-alumina at 25°C, [acetone] = 150 ppm, and [O3] = 1200 ppm, catalyst weight= 0.065 g, gas flow rate= 250 mL?min-1.
Fig.7  DRIFTS spectra of catalytic ozonation of acetone at 25°C using alumina supported (a) Mn10%, (b) Co10% , (c) Mn10%-Co2.5%, and (d) Co10%-Mn2.5%; [acetone] = 150 ppm, [O3] = 1200 ppm, catalyst weight= 0.065 g, gas flow rate= 250 mL?min1.
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