Solid-state interactions, adsorption sites and functionality of Cu-ZnO/ZrO2 catalysts in the CO2 hydrogenation to CH3OH

被引：386

作者：

Arena, Francesco ^{[1
,2
]}

Italiano, Giuseppe ^{[1
]}

Barbera, Katia ^{[3
,4
]}

Bordiga, Silvia ^{[3
,4
]}

Bonura, Giuseppe ^{[2
]}

Spadaro, Lorenzo ^{[2
]}

Frusteri, Francesco ^{[2
]}

机构：

[1] Univ Messina, Dipartimento Chim Ind & Ingn Mat, I-98166 Messina, Italy

[2] Ist CNR ITAE Nicola Giordano, I-98126 Messina, Italy

[3] Univ Turin, Dipartimento Chim Inorgan Fis & Mat, NIS Ctr Excellence, I-10125 Turin, Italy

[4] Univ Turin, Ctr Riferimento INSTM, I-10125 Turin, Italy

来源：

APPLIED CATALYSIS A-GENERAL | 2008年 / 350卷 / 01期

关键词：

Cu-ZnO/ZrO2; catalysts; Solid-state interaction; Adsorption properties; Surface sites; Metal dispersion; Oxide/metal interface; CO2; hydrogenation; Methanol;

D O I：

10.1016/j.apcata.2008.07.028

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：

Structure, adsorption properties and surface reactivity of Cu-ZnO/ZrO2 catalysts (ZrO2 loading, 43 wt%; Zn/Cu (at/at), 0.0-2.8) have been probed by BET, XRD, TPR, N2O-titration, FTIR and TPD measurements of H2, CO and CO2. Characterization data indicate that ZnO promotes the dispersion and reactivity of metal copper to oxygen, while both ZnO and ZrO2 support markedly enhance the surface CO2 adsorption. A synergism of metal Cu hydrogenation and oxide basic sites discloses the primary role of the metal/oxide interface on the functionality of Cu-ZnO/ZrO2 catalysts in the CO2 to CH3OH hydrogenation reaction. The extent of the oxide/metal interface, probed both by Cuδ+/Cu0 and oxide-to-metal surface area (OSA/MSA) ratios, provides a normalization of the Cu site specific activity (TOF) in a wide range (3-60%) of metal dispersion proving the dual-site nature and, then, the formal structure-insensitive character of the title reaction. © 2008 Elsevier B.V. All rights reserved.

引用

页码：16 / 23

页数：8

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