Importance of the Metal-Oxide Interface in Catalysis: In Situ Studies of the Water-Gas Shift Reaction by Ambient-Pressure X-ray Photoelectron Spectroscopy

被引：293

作者：

Mudiyanselage, Kumudu ^{[1
]}

Senanayake, Sanjaya D. ^{[1
]}

Feria, Leticia ^{[2
]}

Kundu, Shankhamala ^{[1
]}

Baber, Ashleigh E. ^{[1
]}

Graciani, Jesus ^{[1
,2
]}

Vidal, Alba B. ^{[1
]}

Agnoli, Stefano ^{[1
]}

Evans, Jaime ^{[3
]}

Chang, Rui ^{[4
]}

Axnanda, Stephanus ^{[5
]}

Liu, Zhi ^{[5
]}

Sanz, Javier F. ^{[2
]}

Liu, Ping ^{[1
]}

Rodriguez, Jose A. ^{[1
]}

Stacchiola, Dario J. ^{[1
]}

机构：

[1] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA

[2] Univ Seville, Dept Quim Fis, E-41012 Seville, Spain

[3] Cent Univ Venezuela, Fac Ciencias, Caracas 1020A, Venezuela

[4] Shanghai Inst Microsyst & Informat Technol, Shanghai 200050, Peoples R China

[5] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2013年 / 52卷 / 19期

关键词：

ceria; heterogeneous catalysis; nanocatalysis; surface chemistry; watergas shift reaction; SURFACE-CHEMISTRY; MECHANISM; CO2; PHOTOEMISSION; CEOX/CU(111); ADSORPTION; OXIDATION; AU(111); COPPER;

D O I：

10.1002/anie.201210077

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Where oxide and metals meet: The activation of an efficient associative mechanistic pathway for the water-gas shift reaction by an oxide-metal interface leads to an increase in the catalytic activity of nanoparticles of ceria deposited on Cu(111) or Au(111) by more than an order of magnitude (see graph). In situ experiments demonstrated that a carboxy species formed at the metal-oxide interface is the critical intermediate in the reaction. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

引用

页码：5101 / 5105

页数：5

共 35 条

[1]

[Anonymous], 1967, ANGEW CHEM INT ED EN, V6, P375

[2]

[Anonymous], 2007, ANGEW CHEM INT ED, V46, P1329

[3] Gold catalysts for pure hydrogen production in the water-gas shift reaction: activity, structure and reaction mechanism [J].

Burch, Robbie .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2006, 8 (47) :5483-5500

[4] A critical analysis of the experimental evidence for and against a formate mechanism for high activity water-gas shift catalysts [J].

Burch, Robbie ;

Goguet, Alexandre ;

Meunier, Frederic C. .

APPLIED CATALYSIS A-GENERAL, 2011, 409 :3-12

[5] Surface chemistry of Cu in the presence of CO2 and H2O [J].

Deng, Xingyi ;

Verdaguer, Albert ;

Herranz, Tirma ;

Weis, Christoph ;

Bluhm, Hendrik ;

Salmeron, Miquel .

LANGMUIR, 2008, 24 (17) :9474-9478

[6] Reactivity Differences of Nanocrystals and Continuous Films of α-Fe2O3 on Au(111) Studied with In Situ X-ray Photoelectron Spectroscopy [J].

Deng, Xingyi ;

Lee, Junseok ;

Wang, Congjun ;

Matranga, Christopher ;

Aksoy, Funda ;

Liu, Zhi .

JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (51) :22619-22623

[7] Effect of the exchange-correlation potential and of surface relaxation on the description of the H2O dissociation on Cu(111) [J].

Fajin, Jose L. C. ;

Illas, Francesc ;

Gomes, Jose R. B. .

JOURNAL OF CHEMICAL PHYSICS, 2009, 130 (22)

[8] Surface chemistry of carbon dioxide [J].

Freund, HJ ;

Roberts, MW .

SURFACE SCIENCE REPORTS, 1996, 25 (08) :225-273

[9] On the mechanism of low-temperature water gas shift reaction on copper [J].

Gokhale, Amit A. ;

Dumesic, James A. ;

Mavrikakis, Manos .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (04) :1402-1414

[10] New ambient pressure photoemission endstation at Advanced Light Source beamline 9.3.2 [J].

Grass, Michael E. ;

Karlsson, Patrik G. ;

Aksoy, Funda ;

Lundqvist, Mans ;

Wannberg, Bjorn ;

Mun, Bongjin S. ;

Hussain, Zahid ;

Liu, Zhi .

REVIEW OF SCIENTIFIC INSTRUMENTS, 2010, 81 (05)

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