Fluorination of dichlorodifluoromethane to synthesize tetrafluoromethane over Cr2O3-AlF3 catalyst

Wenzhi Jia; Lingyun Jin; Yuejuan Wang; Jiqing Lu; Mengfei Luo

Journal of Industrial and Engineering Chemistry, Vol.17, No.3, 615-620, May, 2011

DOI10.1016/j.jiec.2011.05.005 Export Citation

Fluorination of dichlorodifluoromethane to synthesize tetrafluoromethane over Cr2O3-AlF3 catalyst

Wenzhi Jia, Lingyun Jin, Yuejuan Wang, Jiqing Lu, and Mengfei Luo^†

Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China

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A series of Cr2O3-AlF3 catalysts with different Cr2O3 contents were prepared by a deposition. precipitation method for the fluorination of dichlorodifluoromethane (CCl2F2) to synthesize tetrafluoromethane (CF4). The highest activity was obtained on the Cr2O3.AlF3 catalyst containing 61.2 wt.% of Cr2O3, with the CF4 yield of 94% at 400 ℃. X-ray diffraction (XRD) and Raman spectroscopy results indicated the presence of bulk Cr2O3 and a-AlF3 phases in the catalysts. Ammonia temperature programmed desorption (NH3-TPD) and Fourier transformation infrared spectroscopy (FTIR) of pyridine chemisorption revealed strong Lewis acidity of the catalysts. The Cr species and Lewis acid in the Cr2O3-AlF3 catalysts were the active sites of fluorination and dismutation reaction of CCl2F2, respectively. This indicated bi-function catalytic performance of Cr2O3-AlF3 catalysts for fluorination and dismutation reaction.

Keywords:Cr2O3-AlF3 catalyst;CF4;CCl2F2;Fluorination;Lewis acidity;Cr species

[References]

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[1] United Nations Environmental Programme, Report of the Ad Hoc Technical Advisory Committee on ODS Destruction Technologies (1992)

[2] Lee H, Jeong HD, Chung YS, Lee HG, Chung MJ, Kim S, Kim HS, J. Catal., 169(1), 307 (1997)

[3] Hammoudeh A, Mahmoud SS, Gharaibeh S, Appl. Catal. A: Gen., 243(1), 147 (2003)

[4] Kemnitz E, Grob U, Ru¨ diger S, Shekar CS, Angew. Chem. Int. Ed., 42, 4251 (2003)

[5] Ocal M, Maciejewski M, Baiker A, Appl. Catal. B: Environ., 21(4), 279 (1999)

[6] Kemnitz E, Kohne A, Lieske E, J. Fluorine Chem., 81, 197 (1997)

[7] Takita Y, Moriyama J, Nishiguchi H, Ishihara T, Hayano F, Nakajo T, Catal. Today, 88(3-4), 103 (2004)

[8] Williams K, Gupta K, Wasilik M, J. Microelectromech. Syst., 12, 761 (2003)

[9] Kobayashi H, Takaichi T, Hirayama S, EP 366,797 [P] (1990)

[10] Kohne A, Kemnitz E, J. Fluorine Chem., 75, 103 (1995)

[11] Alonso C, Morato A, Medina F, Cesteros Y, Salagre P, Sueiras JE, Appl. Catal. B: Environ., 40(4), 259 (2003)

[12] Young RA, The Rietveld Method, Oxford Univ. Press, Oxford, 22 (1993)

[13] Kemnitz E, Hansen G, Hess A, Kohne A, J. Mol. Catal., 77, 193 (1992)

[14] Yim SD, Nam IS, J. Catal., 221(2), 601 (2004)

[15] Kemnitz E, Menz DH, Prog. Solid State Chem., 26, 97 (1998)

[16] Rao JM, Sivaprasad A, Rao PS, Narsaiah B, Reddy SN, Vijayakumar V, Manorama SV, Krishna KL, Srinivas K, Krishnan KR, Badrinarayanan S, J. Catal., 184(1), 105 (1999)

[17] Albonetti S, Forni L, Cuzzato P, Alberani P, Zappoli S, Trifiro F, Appl. Catal. A: Gen., 326(1), 48 (2007)

[18] Kim DS, Wachs IE, J. Catal., 142, 166 (1993)

[19] Mougin J, Bihan TL, Lucazeau G, J. Phys. Chem. Solids., 62, 553 (2001)

[20] Guo M, Lu JQ, Bi QY, Luo MF, ChemPhysChem., 11, 1693 (2010)

[21] Brown SD, Gard GL, Loehr TM, J. Chem. Phys., 64, 1219 (1976)

[22] Maslar JE, Hurst WS, Bowers WJ, Hendricks JH, Aquino MI, Levin I, Appl. Surf. Sci., 180(1-2), 102 (2001)

[23] He J, Xie GQ, Lu JQ, Qian L, Zhang XL, Fang P, Pu ZY, Luo MF, J. Catal., 253(1), 1 (2008)

[24] Rao JM, Sivaprasad A, Rao PS, Narsaiah B, Reddy SN, Vijayakumar V, Manorama SV, Krishna KL, Srinivas K, Krishnan KR, Badrinarayanan S, J. Catal., 184(1), 105 (1999)

[25] Wojciechowska M, Lomnicki S, Goslar J, Z. Phys. Chem., 189, 113 (1995)

[26] Busca G, Catal. Today, 27(3-4), 323 (1996)

[27] Cho DH, Kim YG, Chung MJ, Chung JS, Appl. Catal. B: Environ., 18(3-4), 251 (1998)

[28] Adamczyk B, Boese O, Weiher N, Schroeder SLM, Kemnitz E, J. Fluorine Chem., 101, 239 (2000)

[29] Unveren E, Kemnitz E, Lippitz A, Unger WES, J. Phys. Chem. B, 109(5), 1903 (2005)