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

[1] Atomic Structure and Special Reactivity Toward Methanol Oxidation of Vanadia Nanoclusters on TiO2(110) [J].

Artiglia, Luca ;

Agnoli, Stefano ;

Vittadini, Andrea ;

Verdini, Alberto ;

Cossaro, Albano ;

Floreano, Luca ;

Granozzi, Gaetano .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (46) :17331-17338

[2] The effect of support on redox properties and methanol-oxidation activity of vanadia catalysts [J].

Baldychev, Ivan ;

Vohs, John M. ;

Gorte, Raymond J. .

APPLIED CATALYSIS A-GENERAL, 2011, 391 (1-2) :86-91

[3] Adsorption of methanol on TiO2(110):: A first-principles investigation [J].

Bates, SP ;

Gillan, MJ ;

Kresse, G .

JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (11) :2017-2026

[4] A synchrotron study of the deposition of vanadia on TiO2(110) [J].

Biener, J ;

Bäumer, M ;

Madix, RJ .

SURFACE SCIENCE, 1999, 432 (03) :178-188

[5] REACTIVITY OF SUPPORTED VANADIUM-OXIDE CATALYSTS - THE PARTIAL OXIDATION OF METHANOL [J].

DEO, G ;

WACHS, IE .

JOURNAL OF CATALYSIS, 1994, 146 (02) :323-334

[6] The surface science of titanium dioxide [J].

Diebold, U .

SURFACE SCIENCE REPORTS, 2003, 48 (5-8) :53-229

[7] Oxidation of methanol to formaldehyde on supported vanadium oxide catalysts compared to gas phase molecules [J].

Döbler, J ;

Pritzsche, M ;

Sauer, J .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (31) :10861-10868

[8] Different binding sites for methanol dehydrogenation and deoxygenation on stoichiometric and defective TiO2(110) surfaces [J].

Farfan-Arribas, E ;

Madix, RJ .

SURFACE SCIENCE, 2003, 544 (2-3) :241-260

[9] A theoretical investigation of the selective oxidation of methanol to formaldehyde on isolated vanadate species supported on titania [J].

Goodrow, Anthony ;

Bell, Alexis T. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (34) :13204-13214

[10] The chemistry of methanol on the surface:: the TiO2 (110) influence of vacancies and coadsorbed species [J].

Henderson, MA ;

Otero-Tapia, S ;

Castro, ME .

FARADAY DISCUSSIONS, 1999, 114 :313-329

← 1 2 3 →