The concentration of oxygen species over SiO2-supported Rh and Ru catalysts and its relationship with the mechanism of partial oxidation of methane to synthesis gas

作者: Wei Zheng Weng , Qian Gu Yan , Chun Rong Luo , Yuan Yan Liao , Hui Lin Wan

DOI: 10.1023/A:1016614510422

关键词:

摘要: The partial oxidation of methane (POM) to synthesis gas over SiO2-supported Rh and Ru catalysts was studied by in situ microprobe Raman time-resolved FTIR (TR-FTIR) spectroscopies. results spectroscopic characterization indicated that no band Rh2O3 detected at 500 °C the Rh/SiO2 catalyst under a flow CH4/O2/Ar (2/1/45, molar ratio) mixture, while bands RuO2 can even be 600°C Ru/SiO2 same atmosphere. experiments TR-FTIR characterizations on reactions CH4 O2 pre-treated products greatly depend concentration O2− species catalysts. On with high O2−, will completely oxidized CO2. However, if is low enough, selectively converted CO without formation parallel using spectroscopy monitor reaction mixture show mechanisms two are quite different. catalyst, mainly formed direct CH4, dominant pathway via sequence total followed reforming unconverted CO2 H2O. significant difference well related conditions due oxygen affinity metals.

参考文章(16)
Y. Boucouvalas, Z.L. Zhang, A.M. Efstathiou, X.E. Verykios, Partial oxidation of methane to synthesis gas over Ru/TiO2 catalysts Studies in Surface Science and Catalysis. ,vol. 101, pp. 443- 452 ,(1996) , 10.1016/S0167-2991(96)80255-2
Wei Zheng Weng, Ming Shu Chen, Qian Gu Yan, Ting Hua Wu, Zi Sheng Chao, Yuan Yan Liao, Hui Lin Wan, Mechanistic study of partial oxidation of methane to synthesis gas over supported rhodium and ruthenium catalysts using in situ time-resolved FTIR spectroscopy Catalysis Today. ,vol. 63, pp. 317- 326 ,(2000) , 10.1016/S0920-5861(00)00475-2
O. V. Buyevskaya, K. Walter, D. Wolf, M. Baerns, Primary reaction steps and active surface sites in the rhodium-catalyzed partial oxidation of methane to CO and H 2 Catalysis Letters. ,vol. 38, pp. 81- 88 ,(1996) , 10.1007/BF00806904
D.D. Beck, T.W. Capehart, C. Wong, D.N. Belton, XAFS Characterization of Rh/Al2O3 After Treatment in High-Temperature Oxidizing Environments Journal of Catalysis. ,vol. 144, pp. 311- 324 ,(1993) , 10.1006/JCAT.1993.1332
C. Elmasides, D. I. Kondarides, W. Grünert, X. E. Verykios, XPS and FTIR Study of Ru/Al2O3 and Ru/TiO2 Catalysts: Reduction Characteristics and Interaction with a Methane−Oxygen Mixture Journal of Physical Chemistry B. ,vol. 103, pp. 5227- 5239 ,(1999) , 10.1021/JP9842291
S.Y. Mar, C.S. Chen, Y.S. Huang, K.K. Tiong, Characterization of RuO2 thin films by Raman spectroscopy Applied Surface Science. ,vol. 90, pp. 497- 504 ,(1995) , 10.1016/0169-4332(95)00177-8
Y.S. Huang, P.C. Liao, Preparation and characterization of RuO2 thin films Solar Energy Materials and Solar Cells. ,vol. 55, pp. 179- 197 ,(1998) , 10.1016/S0927-0248(98)00057-9