Resolving the Atomic Structure of Vanadia Monolayer Catalysts: Monomers, Trimers, and Oligomers on Ceria

被引:148
作者
Baron, Martin [2 ]
Abbott, Heather [2 ]
Bondarchuk, Oleksandr [2 ]
Stacchiola, Dario [2 ]
Uhl, Alexander [2 ]
Shaikhutdinov, Shamil [2 ]
Freund, Hans-Joachim [2 ]
Popa, Cristina [1 ]
Ganduglia-Pirovano, Maria Veronica [1 ]
Sauer, Joachim [1 ]
机构
[1] Humboldt Univ, Dept Chem, D-10009 Berlin, Germany
[2] Max Planck Gesell, Fritz Haber Inst, Dept Chem Phys, D-14195 Berlin, Germany
关键词
density functional calculations; nanoparticles; structure elucidation; surface chemistry; thin films; METAL-OXIDE CATALYSTS; RAMAN-SPECTROSCOPY; THIN-FILMS; OXIDATIVE DEHYDROGENATION; ELECTRONIC-STRUCTURE; MODEL SYSTEMS; CEO2(111); SUPPORT; SILICA; REACTIVITY;
D O I
10.1002/anie.200903085
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
On top of old ceria: Vanadyl-terminated monomers, trimers (see picture), and oligomers form on a CeO2(111) surface, and their atomic structure is resolved using a combination of high-level experimental and theoretical results. Ceria surfaces stabilize vanadia species in a +5 oxidation state, which wet and chemically reduce the ceria surface and probably play a crucial role in the reactivity of ceria-supported vanadia in oxidation reactions. © 2009 Wiley-VCH Verlag.
引用
收藏
页码:8006 / 8009
页数:4
相关论文
共 45 条
[1]  
Banares M. A., 2000, STUD SURF SCI CATAL, V130, P3125, DOI DOI 10.1016/S0167-2991(00)80502-9
[2]   Structural Characterization of Operating Catalysts by Raman Spectroscopy [J].
Banares, Miguel A. ;
Mestl, Gerhard .
ADVANCES IN CATALYSIS, VOL 52, 2009, 52 :43-128
[3]   Interaction of Gold with Cerium Oxide Supports: CeO2(111) Thin Films vs CeOx Nanoparticles [J].
Baron, M. ;
Bondarchuk, O. ;
Stacchiola, D. ;
Shaikhutdinov, S. ;
Freund, H. -J. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (15) :6042-6049
[4]   Surface metal-insulator transition on a vanadium pentoxide (001) single crystal [J].
Blum, R. -P ;
Niehus, H. ;
Hucho, C. ;
Fortrie, R. ;
Ganduglia-Pirovano, M. V. ;
Sauer, J. ;
Shaikhutdinov, S. ;
Freund, H. -J. .
PHYSICAL REVIEW LETTERS, 2007, 99 (22)
[5]   Periodic density functional study on structural and vibrational properties of vanadium oxide aggregates -: art. no. 165420 [J].
Brázdová, V ;
Ganduglia-Pirovano, MV ;
Sauer, J .
PHYSICAL REVIEW B, 2004, 69 (16) :165420-1
[6]   A periodic model for the V2O5-TiO2 (anatase) catalyst.: Stability of dimeric species [J].
Calatayud, M ;
Mguig, B ;
Minot, C .
SURFACE SCIENCE, 2003, 526 (03) :297-308
[7]   Hybrid functionals applied to rare-earth oxides: The example of ceria [J].
Da Silva, Juarez L. F. ;
Ganduglia-Pirovano, M. Veronica ;
Sauer, Joachim ;
Bayer, Veronika ;
Kresse, Georg .
PHYSICAL REVIEW B, 2007, 75 (04)
[8]  
DEO G, 1994, CRIT REV SURF CHEM, V4, P141
[9]   Thermal reduction of vanadium pentoxide: an XPD study [J].
Devriendt, K ;
Poelman, H ;
Fiermans, L .
SURFACE SCIENCE, 1999, 433 :734-739
[10]   Vibrations of Silica Supported Vanadia: Variation with Particle Size and Local Surface Structure [J].
Doebler, Jens ;
Pritzsche, Marc ;
Sauer, Joachim .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (28) :12454-12464