Methane oxidation to formaldehyde over vanadium oxide supported on various mesoporous silicas

Euiseob Yang; Jun Gyeong Lee; Eun Duck Park; Kwangjin An

Korean Journal of Chemical Engineering, Vol.38, No.6, 1224-1230, June, 2021

DOI10.1007/s11814-021-0758-8 Export Citation

Methane oxidation to formaldehyde over vanadium oxide supported on various mesoporous silicas

Euiseob Yang, Jun Gyeong Lee, Eun Duck Park^{1, †}, and Kwangjin An^†

School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Korea
¹Department of Chemical Engineering and Department of Energy Systems Research, Ajou University, Suwon 16499, Korea

E-mail:,

To investigate the role of vanadium oxide supported on mesoporous silica (VOx/m-SiO2) catalysts in methane oxidation to formaldehyde, various catalysts were prepared. The type of m-SiO2 (SBA-15 and MCF-17), vanadium loading (1, 3, and 5%), and preparation method (wet impregnation; WI and dry impregnation; DI) were changed to produce VOx/m-SiO2 with different vanadium species. Because of the larger surface area and pore size, a higher dispersion of vanadium loading, 1% VOx/MCF-17(DI), showed the highest conversion (20.2%) in methane oxidation at 600 °C. Various characterizations revealed that DI was a better method to produce isolated tetrahedral monovanadate species in VOx/m-SiO2 catalysts than WI. As the vanadium loading was decreased from 5 to 1%, the methane conversion was further increased due to the higher degree of dispersion of monomeric VO4 generated in the catalysts with low vanadium loading. The combined results demonstrate that the dispersion of vanadium and the isolated monomeric VO4 phase increased when the vanadium catalyst was loaded on MCF-17 and prepared by the DI method.

Keywords:Vanadium;Mesoporous Silica;Methane Oxidation;Formaldehyde;Dry Impregnation

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[3] Ohler N, Bell AT, J. Phys. Chem. B, 110(6), 2700 (2006)

[4] Lunsford JH, Catal. Today, 63(2-4), 165 (2000)

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[6] Monai M, Montini T, Gorte RJ, Fornasiero P, Eur. J. Inorg. Chem., 25, 2884 (2018)

[7] Nguyen LD, Loridant S, Launay H, Pigamo A, Dubois JL, Millet JMM, J. Catal., 237(1), 38 (2006)

[8] Arena F, Parmaliana A, Accounts Chem. Res., 36, 867 (2003)

[9] Du GA, Lim SY, Yang YH, Wang C, Pfefferle L, Haller GL, Appl. Catal. A: Gen., 302(1), 48 (2006)

[10] Hutchings GJ, Scurrell MS, Woodhouse JR, Chem. Soc. Rev., 18, 251 (1989)

[11] Herman RG, Sun Q, Shi CL, Klier K, Wang CB, Hu HC, Wachs IE, Bhasin MM, Catal. Today, 37(1), 1 (1997)

[12] Parmaliana A, Sokolovskii V, Miceli D, Arena F, Giordano N, ACS Symp. Ser., Am. Chem. Soc., Washington, DC, 43 (1993).

[13] Sun XH, Shi YF, Zhang P, Zheng CM, Zheng XY, Zhang F, Zhang YC, Guan NJ, Zhao DY, Stucky GD, J. Am. Chem. Soc., 133(37), 14542 (2011)

[14] Perego C, Millini R, Chem. Soc. Rev., 42, 3956 (2013)

[15] Gu D, Schuth F, Chem. Soc. Rev., 43, 313 (2014)

[16] Wallis P, Wohlrab S, Kalevaru VN, Frank M, Martin A, Catal. Today, 278, 120 (2016)

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[19] Schwarz JA, Contescu C, Contescu A, Chem. Rev., 95(3), 477 (1995)

[20] Zhao D, Sun J, Li Q, Stucky GD, Chem. Mater., 12, 275 (2000)

[21] Klimova T, Esquivel A, Reyes J, Rubio M, Bokhimi X, Aracil J, Microporous Mesoporous Mater., 93, 331 (2006)

[22] Tsung CK, Kuhn JN, Huang WY, Aliaga C, Hung LI, Somorjai GA, Yang PD, J. Am. Chem. Soc., 131(16), 5816 (2009)

[23] Siggia S, Maxcy W, Anal. Chem., 19, 1023 (1947)

[24] Sugino T, Kido A, Azuma N, Ueno A, Udagawa Y, J. Catal., 190(1), 118 (2000)

[25] Carrero CA, Schloegl R, Wachs IE, Schomaecker R, ACS Catal., 4, 3357 (2014)

[26] Du G, Lim S, Pinault M, Wang C, Fang F, Pfefferle L, Haller GL, J. Catal., 253(1), 74 (2008)

[27] Olthof B, Khodakov A, Bell AT, Iglesia E, J. Phys. Chem. B, 104(7), 1516 (2000)

[28] Wei D, Wang H, Feng XB, Chueh WT, Ravikovitch P, Lyubovsky M, Li C, Takeguchi T, Haller GL, J. Phys. Chem. B, 103(12), 2113 (1999)

[29] Sokolovskii V, Arena F, Coluccia S, Parmaliana A, J. Catal., 173(1), 238 (1998)

[30] Gao XT, Wachs IE, J. Phys. Chem. B, 104(6), 1261 (2000)

[31] Burcham LJ, Deo G, Gao X, Wachs IE, Top. Catal., 11, 85 (2000)

[32] Gao XT, Bare SR, Weckhuysen BM, Wachs IE, J. Phys. Chem. B, 102(52), 10842 (1998)

[33] Launay H, Loridant S, Pigamo A, Dubois JL, Millet JMM, J. Catal., 246(2), 390 (2007)

[34] Keller DE, Visser T, Soulimani F, Koningsberger DC, Weckhuysen BM, Vib. Spectrosc., 43, 140 (2007)

[35] Weckhuysen BM, Keller DE, Catal. Today, 78(1-4), 25 (2003)

[36] Anshits AG, Kondratenko EV, Voskresenskaya EN, Kurteeva LI, Pavlenko NI, Catal. Today, 46(2-3), 211 (1998)

[37] Deegan RD, Bakajin O, Dupont TF, Huber G, Nagel SR, Witten TA, Nature, 389(6653), 827 (1997)

[38] Kumar S, Katz JS, Schroeder CM, Phys. Rev. Fluid, 2, 114304 (2017)