CO2 hydrogenation at low temperature over Rh/gamma-Al2O3 catalysts: effect of the metal particle size on catalytic performances and reaction mechanism
作者： Alejandro Karelovic , Patricio Ruiz
DOI: 10.1016/J.APCATB.2011.11.043
关键词: Reaction mechanism 、 Catalysis 、 Particle size 、 Methanation 、 Dissociation (chemistry) 、 Inorganic chemistry 、 Diffuse reflectance infrared fourier transform 、 Rhodium 、 Chemistry 、 Activation energy
摘要: Low temperature CO2 methanation was studied on Rh/γ-Al2O3 catalysts. Catalysts were prepared with varying amounts of Rh to obtain different mean particle sizes, ranging between 3.6 and 15.4 nm. In the conditions studied, selectivity methane 100%. The intrinsic activity catalysts in hydrogenation found do not depend size at temperatures 185 200 °C, whereas lower larger particles favored higher activity. Apparent activation energies be range 14.5–22.7 kcal/mol. Lower obtained for particles. Operando-DRIFTS (Diffuse Reflectance Infrared Fourier Transform Spectroscopy) experiments showed that is readily dissociated these 50 °C giving rise carbonyl formates species. Rh–CO species are proposed associated H forming hydrides. According transient performed gas atmospheres, it adsorbed CO an important intermediate spectators reaction path. Activation energy dissociation similar overall which suggests importance bond
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sci-hub.se 参考文章(53)
Yoshihiko Mori, Toshiaki Mori, Akira Miyamoto, Naoki Takahashi, Tadashi Hattori, Yuichi Murakami, Support effect on surface reaction rates in CO hydrogenation over supported Rh catalysts The Journal of Physical Chemistry. ,vol. 93, pp. 2039- 2043 ,(1989) , 10.1021/J100342A065
M. Albert Vannice, Kinetics of Catalytic Reactions ,(2005)
H. Wijnja, C.P. Schulthess, ATR–FTIR and DRIFT spectroscopy of carbonate species at the aged γ-Al2O3/water interface Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy. ,vol. 55, pp. 861- 872 ,(1999) , 10.1016/S1386-1425(98)00236-4
Paraskevi Panagiotopoulou, Dimitris I. Kondarides, Xenophon. E. Verykios, Selective methanation of CO over supported Ru catalysts Applied Catalysis B-environmental. ,vol. 88, pp. 470- 478 ,(2009) , 10.1016/J.APCATB.2008.10.012
Michel Marwood, Ralf Doepper, Michael Prairie, Albert Renken, Transient drift spectroscopy for the determination of the surface reaction kinetics of CO2 methanation Chemical Engineering Science. ,vol. 49, pp. 4801- 4809 ,(1994) , 10.1016/S0009-2509(05)80060-0
Marc Jacquemin, Antoine Beuls, Patricio Ruiz, Catalytic production of methane from CO2 and H2 at low temperature: insight on the reaction mechanism Catalysis Today. ,vol. 157, pp. 462- 466 ,(2010) , 10.1016/J.CATTOD.2010.06.016
Gordon D Weatherbee, Calvin H Bartholomew, Hydrogenation of CO2 on group VIII metals II. Kinetics and mechanism of CO2 hydrogenation on nickel Journal of Catalysis. ,vol. 77, pp. 460- 472 ,(1982) , 10.1016/0021-9517(82)90186-5
P.B. Rasband, W.C. Hecker, Catalyst Characterization Using Quantitative FTIR: CO on Supported Rh Journal of Catalysis. ,vol. 139, pp. 551- 560 ,(1993) , 10.1006/JCAT.1993.1048
J.H. Scofield, Hartree-Slater subshell photoionization cross-sections at 1254 and 1487 eV Journal of Electron Spectroscopy and Related Phenomena. ,vol. 8, pp. 129- 137 ,(1976) , 10.1016/0368-2048(76)80015-1
J. C. Lavalley, J. Saussey, J. Lamotte, R. Breault, J. P. Hindermann, A. Kiennemann, Infrared study of carbon monoxide hydrogenation over rhodium/ceria and rhodium/silica catalysts The Journal of Physical Chemistry. ,vol. 94, pp. 5941- 5947 ,(1990) , 10.1021/J100378A061