Catalytic Oxidation of Methanol to Formaldehyde by Mass-Selected Vanadium Oxide Clusters Supported on a TiO2(110) Surface

被引：19

作者：

Price, Scott P. ^{[1
]}

Tong, Xiao ^{[1
]}

Ridge, Claron ^{[1
]}

Neilson, Hunter L. ^{[1
]}

Buffon, Joshua W. ^{[1
]}

Robins, Jeremy ^{[1
]}

Metiu, Horia ^{[1
]}

Bowers, Michael T. ^{[1
]}

Buratto, Steven K. ^{[1
]}

机构：

[1] Univ Calif Santa Barbara, Dept Chem & Biochem, Santa Barbara, CA 93106 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2014年 / 118卷 / 37期

基金：

美国国家科学基金会;

关键词：

RUTILE TIO2(110); REACTIVITY; OXYGEN; DEPOSITION; CHEMISTRY; SCIENCE; FILMS;

D O I：

10.1021/jp5011378

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：

We report the results of a systematic study of the catalytic activity of mass-selected vanadium oxide dusters deposited on rutile TiO2 surfaces under ultrahigh vacuum (UHV) conditions. Our results show that supported V. VO, and VO2 clusters are not catalytically active for the oxidative dehydrogenation of methanol to formaldehyde but can be made catalytically active by postoxidation. In addition, we found that the postoxidized VO/TiO2 produces the most formaldehyde. Scanning tunneling microscopy (STM) imaging of the postoxidized VO/TiO2 reveals isolated dusters with height and width indicative of VO3 bound to the TiO2 surface. Our results are consistent with previous density functional theory (DFT) calculations that predict that VO3 will be produced by postoxidation of VO and that VO3/TiO2 is an active catalyst.

引用

页码：8309 / 8313

页数：5

共 24 条

[11] Formation, deposition and examination of size selected metal clusters on semiconductor surfaces: An experimental setup [J].

Kemper, Paul ;

Kolmakov, Andrei ;

Tong, Xiao ;

Lilach, Yigal ;

Benz, Lauren ;

Manard, Manuel ;

Metiu, Horia ;

Buratto, Steven K. ;

Bowers, Michael T. .

INTERNATIONAL JOURNAL OF MASS SPECTROMETRY, 2006, 254 (03) :202-209

[12] Oxidative Dehydrogenation of Methanol to Formaldehyde by a Vanadium Oxide Cluster Supported on Rutile TiO2(110): Which Oxygen is Involved? [J].

Kim, Hyun You ;

Lee, Hyuck Mo ;

Metiu, Horia .

JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (32) :13736-13738

[13] Oxygen-induced restructuring of the TiO2(110) surface:: a comprehensive study [J].

Li, M ;

Hebenstreit, W ;

Gross, L ;

Diebold, U ;

Henderson, MA ;

Jennison, DR ;

Schultz, PA ;

Sears, MP .

SURFACE SCIENCE, 1999, 437 (1-2) :173-190

[14] Interaction of CO2 with oxygen adatoms on rutile TiO2(110) [J].

Lin, Xiao ;

Wang, Zhi-Tao ;

Lyubinetsky, Igor ;

Kay, Bruce D. ;

Dohnalek, Zdenek .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (17) :6190-6195

[15] Observation of All the Intermediate Steps of a Chemical Reaction on an Oxide Surface by Scanning Tunneling Microscopy [J].

Matthiesen, Jesper ;

Wendt, Stefan ;

Hansen, Jonas O. ;

Madsen, Georg K. H. ;

Lira, Estephania ;

Galliker, Patrick ;

Vestergaard, Ebbe K. ;

Schaub, Renald ;

Laegsgaard, Erik ;

Hammer, Bjork ;

Besenbacher, Flemming .

ACS NANO, 2009, 3 (03) :517-526

[16] STM characterization of size-selected V1, V2, VO and VO2 clusters on a TiO2 (110)-(1 x 1) surface at room temperature [J].

Price, Scott P. ;

Tong, Xiao ;

Ridge, Claron ;

Shapovalov, Vladimir ;

Hu, Zhenpeng ;

Kemper, Paul ;

Metiu, Horia ;

Bowers, Michael T. ;

Buratto, Steven K. .

SURFACE SCIENCE, 2011, 605 (9-10) :972-976

[17] VOx (x=1-4) submonolayers supported on rutile TiO2(110) and CeO2(111) surfaces:: The structure, the charge of the atoms, the XPS spectrum, and the equilibrium composition in the presence of oxygen [J].

Shapovalov, Vladimir ;

Metiu, Horia .

JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (38) :14179-14188

[18] Recent conceptual advances in the catalysis science of mixed metal oxide catalytic materials [J].

Wachs, IE .

CATALYSIS TODAY, 2005, 100 (1-2) :79-94

[19] Partial oxidation of methanol to formaldehyde on a model supported monolayer vanadia catalyst:: vanadia on TiO2(110) [J].

Wang, QG ;

Madix, RJ .

SURFACE SCIENCE, 2002, 496 (1-2) :51-63

[20] Preparation and reactions of V2O5 supported on TiO2(110) [J].

Wang, QG ;

Madix, RJ .

SURFACE SCIENCE, 2001, 474 (1-3) :L213-L216

← 1 2 3 →