The Direct Influence of the Support on the Electronic Structure of the Active Sites in Supported Metal Catalysts : Evidence from Pt-H Anti-Bonding Shape Resonance and Pt-CO FTIR Data
作者： D.C. Koningsberger , D.E. Ramaker , J.T. Miller , J. de Graaf , B.L. Mojet
关键词: Physical chemistry 、 Fermi level 、 Valence (chemistry) 、 Metal 、 Infrared spectroscopy 、 Noble metal 、 Chemistry 、 Inorganic chemistry 、 Absorption spectroscopy 、 Neopentane 、 Shape resonance
摘要: The catalytic activity and spectroscopic properties of supported noble metal catalysts are strongly influenced by support such as the presence protons, type charge compensating cations, Si/Al ratio and/or extra-framework Al. metal–support interaction is relatively independent (Pd or Pt) (microporous zeolites LTL Y macroporous supports SiO2). As alkalinity increases (i.e., with increasing electronic on oxygen ions), TOF particles for neopentane hydrogenolysis decreases. At same time, there a systematic shift from linear to bridge bonded CO indicated IR spectra. This strong indication change in structure catalytically active Pt surface atoms. Analysis Pt–H anti-bonding shape resonance present X-ray absorption spectra L3 edge indicates that difference energy between orbital Fermi level decreases increases. results data directly show influences position valence orbitals. ionisation potential atoms alkalinity, i.e., electron ions. leads weakening bond.
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sci-hub.se 参考文章(31)
A. de Mallmann, D. Barthomeuf, Specific Platinum Particles Properties in Basic Zeolites Studies in Surface Science and Catalysis. ,vol. 46, pp. 429- 438 ,(1989) , 10.1016/S0167-2991(08)60999-4
A. P. J. Jansen, R. A. Van Santen, Hartree-Fock-Slater calculations on cation-induced changes in the adsorption of carbon monoxide on iridium tetrameric clusters The Journal of Physical Chemistry. ,vol. 94, pp. 6764- 6772 ,(1990) , 10.1021/J100380A043
D. P. Woodruff, D. A. King, The Chemical Physics of Solid Surfaces and Heterogeneous Catalysis ,(1981)
K. Asakura, T. Kubota, N. Ichikuni, Y. Iwasawa, A new characterization method for adsorbed hydrogen on supported Pt particles Studies in Surface Science and Catalysis. ,vol. 101, pp. 911- 919 ,(1996) , 10.1016/S0167-2991(96)80302-8
B.L. Mojet, D.E. Ramaker, J.T. Miller, D.C. Koningsberger, Observation of a hydrogen-induced shape resonance on Pt/LTL catalysts and its relation with support acidity/alkalinity Catalysis Letters. ,vol. 62, pp. 15- 20 ,(1999) , 10.1023/A:1019018215806
B.L. Mojet, M.J. Kappers, J.C. Muijsers, J.W. Niemantsverdriet, J.T. Miller, F.S. Modica, D.C. Koningsberger, Electronic Modifictions in Supported Palladium Catalysts Studies in Surface Science and Catalysis. ,vol. 84, pp. 909- 916 ,(1994) , 10.1016/S0167-2991(08)63623-X
B.L. Mojet, M.J. Kappers, J.T. Miller, D.C. Koningsberger, Metal-Support Interactions in Supported Platinum Catalysts: Zeolites and Amorphous Supports. Studies in Surface Science and Catalysis. ,vol. 101, pp. 1165- 1174 ,(1996) , 10.1016/S0167-2991(96)80328-4
D.C. Koningsberger, M.K. Oudenhuijzen, J.H. Bitter, D.E. Ramaker, Study of geometrical and electronic effects induced by hydrogen chemisorption on supported Pt particles. Analysis of Pt–H EXAFS and Pt–H anti-bonding state shape resonances Topics in Catalysis. ,vol. 10, pp. 167- 177 ,(2000) , 10.1023/A:1019153226151
R. van Hardeveld, F. Hartog, Influence of Metal Particle Size in Nickel-on-Aerosil Catalysts on Surface Site Distribution, Catalytic Activity, and Selectivity Advances in Catalysis. ,vol. 22, pp. 75- 113 ,(1972) , 10.1016/S0360-0564(08)60246-1
S.D. Lin, M.A. Vannice, Hydrogenation of Aromatic Hydrocarbons over Supported Pt Catalysts .II. Toluene Hydrogenation Journal of Catalysis. ,vol. 143, pp. 554- 562 ,(1993) , 10.1006/JCAT.1993.1298