Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2

被引：1243

作者：

Graciani, Jesus ^{[1
]}

Mudiyanselage, Kumudu ^{[2
]}

Xu, Fang ^{[2
]}

Baber, Ashleigh E. ^{[2
]}

Evans, Jaime ^{[3
]}

Senanayake, Sanjaya D. ^{[2
]}

Stacchiola, Dario J. ^{[2
]}

Liu, Ping ^{[2
]}

Hrbek, Jan ^{[2
]}

Fernandez Sanz, Javier ^{[1
]}

Rodriguez, Jose A. ^{[2
]}

机构：

[1] Univ Seville, Dept Phys Chem, E-41012 Seville, Spain

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

[3] Cent Univ Venezuela, Fac Ciencias, Caracas 10201, Venezuela

来源：

SCIENCE | 2014年 / 345卷 / 6196期

关键词：

GAS SHIFT REACTION; MIXED-METAL OXIDE; NANOMETER LEVEL; IN-SITU; WATER; HYDROGENATION; SURFACES; CU; NANOPARTICLES; SPECTROSCOPY;

D O I：

10.1126/science.1253057

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

The transformation of CO2 into alcohols or other hydrocarbon compounds is challenging because of the difficulties associated with the chemical activation of CO2 by heterogeneous catalysts. Pure metals and bimetallic systems used for this task usually have low catalytic activity. Here we present experimental and theoretical evidence for a completely different type of site for CO2 activation: a copper-ceria interface that is highly efficient for the synthesis of methanol. The combination of metal and oxide sites in the copper-ceria interface affords complementary chemical properties that lead to special reaction pathways for the CO2 -> CH3OH conversion.

引用

页码：546 / 550

页数：5

共 27 条

[1] CO2 activation and promotional effect in the oxidation of cyclic olefins over mesoporous carbon nitrides [J].

Ansari, Mohd Bismillah ;

Min, Byung-Hoon ;

Mo, Yong-Hwan ;

Park, Sang-Eon .

GREEN CHEMISTRY, 2011, 13 (06) :1416-1421

[2]

Aresta M., 2010, CARBON DIOXIDE CHEM

[3] In Situ Imaging of Cu2O under Reducing Conditions: Formation of Metallic Fronts by Mass Transfer [J].

Baber, Ashleigh E. ;

Xu, Fang ;

Dvorak, Filip ;

Mudiyanselage, Kumudu ;

Soldemo, Markus ;

Weissenrieder, Jonas ;

Senanayake, Sanjaya D. ;

Sadowski, Jerzy T. ;

Rodriguez, Jose A. ;

Matolin, Vladimir ;

White, Michael G. ;

Stacchiola, Dario J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (45) :16781-16784

[4]

Behrens M, 2012, SCIENCE, V336, P893, DOI [10.1126/science.1219831, 10.1126/science.12198331]

[5] MECHANISM OF METHANOL SYNTHESIS FROM CO2/CO/H2 MIXTURES OVER COPPER/ZINC OXIDE/ALUMINA CATALYSTS - USE OF C-14-LABELED REACTANTS [J].

CHINCHEN, GC ;

DENNY, PJ ;

PARKER, DG ;

SPENCER, MS ;

WHAN, DA .

APPLIED CATALYSIS, 1987, 30 (02) :333-338

[6] 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

[7] Temperature evolution of structure and bonding of formic acid and formate on fully oxidized and highly reduced CeO2(111) [J].

Gordon, Wesley O. ;

Xu, Ye ;

Mullins, David R. ;

Overbury, Steven H. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2009, 11 (47) :11171-11183

[8] A theoretical insight into the catalytic effect of a mixed-metal oxide at the nanometer level: The case of the highly active metal/CeOx/TiO2(110) catalysts [J].

Graciani, Jesus ;

Plata, Jose J. ;

Fdez Sanz, Javier ;

Liu, Ping ;

Rodriguez, Jose A. .

JOURNAL OF CHEMICAL PHYSICS, 2010, 132 (10)

[9] Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst [J].

Green, Isabel Xiaoye ;

Tang, Wenjie ;

Neurock, Matthew ;

Yates, John T., Jr. .

SCIENCE, 2011, 333 (6043) :736-739

[10] CARBON-MONOXIDE AND CARBON-DIOXIDE ADSORPTION ON CERIUM OXIDE STUDIED BY FOURIER-TRANSFORM INFRARED-SPECTROSCOPY .1. FORMATION OF CARBONATE SPECIES ON DEHYDROXYLATED CEO2 AT ROOM-TEMPERATURE [J].

LI, C ;

SAKATA, Y ;

ARAI, T ;

DOMEN, K ;

MARUYA, K ;

ONISHI, T .

JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1989, 85 :929-943

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