1. Key Lab of Education Ministry on Controlling Chemical Reaction, Beijing University of Chemical Technology, Beijing 100029, China 2. School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200072，China
Abstract：The reaction pathway of n-butane selective oxidation to maleic anhydride (MA) over vanadium phosphorous oxide (VO)2P2O7 catalysts was systematically probed using in situ transient Diffuse Reflectance Infrared Fourier-Transform Spectroscopy (DRIFTS) in high temperature/high pressure chamber. The unsaturated and saturated noncyclic carbonyl species were determined to be intermediates in n-butane selective oxidation to MA. Furan was detected on the surface of the (VO)2P2O7 catalysts in 1-butene, 1, 3-butadiene selective oxidation. It was deduced that furan ring was cleaved to form unsaturated noncyclic carbonyl species before its conversion to MA. Based on these results and in comparison with the literature, a simplified scheme of the reaction network structure can be proposed for n-butane selective oxidation to maleic anhydride.
[1] Coulston G W, Bare S R, Lee P L et al. Science, 1997, 275: 191. [2] Centi G, Triffiro F, Enber J R, Franchetti V M. Chem. Rev.，1988, 88: 55. [3] Contractor R M. Chem. Eng. Sci., 1999，54: 5627. [4] Huang X F, Li C Y, Chen B H et al. Ind. Eng. Chem. Res., 2001, 40: 768. [5] Pekar M, Koubek C M. Chem. Eng. Sci., 1997, 52: 2291. [6] LIANG Ri-zhong et al (梁日忠等). J. Mol. Catal. (China) (分子催化), 2001, 15(2): 86. [7] Wenig R W, Schrader G L. J. Phys. Chem.，1986, 90：6480. [8] Busca G, Centi G. J. Am. Chem. Soc.，1986, 108：46. [9] Busca G, Ramis G, Lorenzelli V. J. Mol. Catal., 1989, 55：1. [10] Ramstetter A, Baerns M. J. Catal., 1988, 109：303. [11] Wenig R W, Schrader G L. J. Phys. Chem.，1987, 91：1911. [12] Wenig R W, Schrader G L. J. Phys. Chem.，1987, 91：5674. [13] Puttock S J, Rochester C H. J. Chem. Soc., Faraday Trans. 1986, 182：3033. [14] Do N T, Barens M. Appl. Catal., 1988, 45：9. [15] Puttock S J, Rochester C H. J. Chem. Soc., Faraday Trans. 1986, 182：3013. [16] Baliamy L J. The Infrared Spectra of Complex Molecules. 2nd. ed. Vol.2, Advances in Infrared Group Frequencies. London：Chapman and Hall, 1980. [17] Nakanishi K, Solomon P H. Infrared Absorption Spectroscopy, Second Edition, oakland CA：Holden-Day, 1977. [18] Davydov A A. Infrared Spectroscopy of Adsorbed Species on the Surface of Transition Metal Oxides, New York：Wiley, 1984. [19] Pouchert C J. The Aldrich Library of FTIR Spectra, Edition 1. Vol. 3, Aldrich Chemical, Co., 1989. [20] Crew W W, Madix R J. J. Am. Chem. Soc., 1993, 115：729. [21] Xue Zhi-Yang，Schrader G L. J. Catal.，1999, 184：87. [22] Centi G, Fornasari G, Trifiro F. J. Catal, 1984, 89: 44. [23] Trimm D L. Design of Industrial Catalysts, New York: Elsevier, 1980.
