In situ FTIR and Raman study on the distribution and reactivity of surface vanadia species in V2O5/CeO2 catalysts

被引:34
作者
Bosco, Marta V. [1 ]
Banares, Miguel A. [2 ]
Martinez-Huerta, Maria V. [2 ]
Bonivardi, Adrian L. [1 ]
Collins, Sebastian E. [1 ]
机构
[1] UNL, CONICET, Inst Desarrollo Tecnol Ind Quim INTEC, RA-3000 Santa Fe, Argentina
[2] CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain
关键词
Vanadia; Ceria; Methanol oxidation; Raman; Infrared spectroscopy; METAL-OXIDE CATALYSTS; METHANOL OXIDATION; INFRARED-SPECTROSCOPY; VIBRATIONAL-SPECTRA; ACTIVE-SITES; CEO2; NANOCRYSTALS; CARBON-DIOXIDE; FORMIC-ACID; ADSORPTION; CERIA;
D O I
10.1016/j.molcata.2015.07.012
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The surface structure and reactivity of vanadia supported on ceria catalysts were studied by Raman spectroscopy and methanol adsorption and temperature-programmed surface reaction (TPRS) of the adsorbed species monitored in situ by infrared spectroscopy. Monomeric and polymeric vanadia surface species and CeVO4 were identified on the catalysts. Methanol adsorption reveled that mostly reduced Ce3+ sites are present in the surface of the catalysts, produced as a result of the reductive solid reaction of VOx species with the ceria surface. Adsorbed methanol/methoxy decomposed stepwise to formate and, finally, carbonate/carbon dioxide. The reactivity is linked to interphase sites, Ce-O-V, which could favor the abstraction of hydrogen during the methoxy transformation to formates. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:75 / 84
页数:10
相关论文
共 66 条
[1]   Relating methanol oxidation to the structure of ceria-supported vanadia monolayer catalysts [J].
Abbott, H. L. ;
Uhl, A. ;
Baron, M. ;
Lei, Y. ;
Meyer, R. J. ;
Stacchiola, D. J. ;
Bondarchuk, O. ;
Shaikhutdinov, S. ;
Freund, H. J. .
JOURNAL OF CATALYSIS, 2010, 272 (01) :82-91
[2]   VIBRATIONAL-SPECTRA AND VALENCE FORCE-FIELD OF CRYSTALLINE V2O5 [J].
ABELLO, L ;
HUSSON, E ;
REPELIN, Y ;
LUCAZEAU, G .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1983, 39 (07) :641-651
[3]   Fundamental, binary combination, and overtone modes in methoxy adsorbed on Cu(100): Infrared spectroscopy and ab initio calculations [J].
Andersson, MP ;
Uvdal, P ;
MacKerell, AD .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (20) :5200-5211
[4]   Methanol: a "smart" chemical probe molecule [J].
Badlani, M ;
Wachs, IE .
CATALYSIS LETTERS, 2001, 75 (3-4) :137-149
[5]   Use of methanol as an IR molecular probe to study the surface of polycrystalline ceria [J].
Badri, A ;
Binet, C ;
Lavalley, JC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (06) :1159-1168
[6]   Molecular structures of supported metal oxide catalysts under different environments [J].
Bañares, MA ;
Wachs, IE .
JOURNAL OF RAMAN SPECTROSCOPY, 2002, 33 (05) :359-380
[7]  
Banares MA, 2000, STUD SURF SCI CATAL, V130, P3125, DOI [10.1016/S0167-2991(00)80502-9, DOI 10.1016/S0167-2991(00)80502-9]
[8]   ORTHOVANADATES AND RELATED COMPOUNDS .2. LANTHANUM ORTHOVANADATES [J].
BARAN, EJ ;
AYMONINO, PJ .
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE, 1971, 383 (02) :220-&
[9]   ORTHO-VANADATES AND RELATED-COMPOUNDS .34. THE VIBRATIONAL-SPECTRA OF INVO4 AND TIVO4 [J].
BARAN, EJ ;
ESCOBAR, ME .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1985, 41 (03) :415-417
[10]   Resolving the Atomic Structure of Vanadia Monolayer Catalysts: Monomers, Trimers, and Oligomers on Ceria [J].
Baron, Martin ;
Abbott, Heather ;
Bondarchuk, Oleksandr ;
Stacchiola, Dario ;
Uhl, Alexander ;
Shaikhutdinov, Shamil ;
Freund, Hans-Joachim ;
Popa, Cristina ;
Ganduglia-Pirovano, Maria Veronica ;
Sauer, Joachim .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (43) :8006-8009