Infrared Evidence of a Formate-Intermediate Mechanism over Ca-Modified Supports in Low-Temperature Ethanol Steam Reforming

被引：31

作者：

Choong, Catherine ^{[1
,2
]}

Zhong, Ziyi ^{[1
]}

Huang, Lin ^{[1
]}

Borgna, Armando ^{[1
]}

Hong, Liang ^{[2
]}

Chen, Luwei ^{[1
]}

Lin, Jianyi ^{[1
]}

机构：

[1] ASTAR, Inst Chem & Engn Sci, Singapore 627833, Singapore

[2] Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore 119260, Singapore

来源：

ACS CATALYSIS | 2014年 / 4卷 / 07期

关键词：

ethanol steam reforming; reaction pathway; acetate; formate; Pt; Rh; Pd; Ca; Al2O3; NOBLE-METAL CATALYSTS; GAS SHIFT REACTION; SITU FT-IR; PROGRAMMED DESORPTION; HYDROGEN-PRODUCTION; SURFACE-REACTIONS; CALCIUM ADDITION; ALUMINUM-OXIDE; RH CATALYSTS; ADSORPTION;

D O I：

10.1021/cs500358n

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：

An in situ DRIFTS study of ethanol adsorption and desorption was performed on Pt (Rh, Pd) supported on Al2O3 and Ca-Al2O3. Different from the well-known acetate-intermediate reaction mechanism observed on Al2O3-supported metal catalysts, formate species are exclusively observed on Pt (Rh, Pd) supported on Ca-Al2O3, offering a new mechanism denoted as the formate-intermediate mechanism. The key factor in determining the change in mechanism is the reduced availability of surface oxygen and the enhanced C-C breaking ability of the metal catalyst upon Ca modification. The formate-intermediate mechanism is favored in the presence of noble metals in the following order: Pt > Rh > Pd.

引用

页码：2359 / 2363

页数：5

共 34 条

[21] Oxygenate reaction pathways on transition metal surfaces [J].

Mavrikakis, M ;

Barteau, MA .

JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1998, 131 (1-3) :135-147

[22] Effect of the nature of the support on the catalytic performance of noble metal catalysts for the water-gas shift reaction [J].

Panagiotopoulou, P ;

Kondarides, DI .

CATALYSIS TODAY, 2006, 112 (1-4) :49-52

[23] Mechanistic aspects of the low temperature steam reforming of ethanol over supported Pt catalysts [J].

Panagiotopoulou, Paraskevi ;

Verykios, Xenophon E. .

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2012, 37 (21) :16333-16345

[24] FTIR and mass spectrometric study of the interaction of ethanol and ethanol-water with oxide-supported platinum catalysts [J].

Raskó, J ;

Dömök, A ;

Baán, K ;

Erdohelyi, A .

APPLIED CATALYSIS A-GENERAL, 2006, 299 (202-211) :202-211

[25] Adsorption and surface reactions of acetaldehyde on TiO2, CeO2 and Al2O3 [J].

Raskó, J ;

Kiss, J .

APPLIED CATALYSIS A-GENERAL, 2005, 287 (02) :252-260

[26] REACTANT-PROMOTED REACTION-MECHANISM FOR CATALYTIC WATER GAS SHIFT REACTION ON MGO [J].

SHIDO, T ;

ASAKURA, K ;

IWASAWA, Y .

JOURNAL OF CATALYSIS, 1990, 122 (01) :55-67

[27] Effect of the metal nature on the reaction mechanism of the partial oxidation of ethanol over CeO2-supported Pt and Rh catalysts [J].

Silva, A. M. ;

Costa, L. O. O. ;

Barandas, A. P. M. G. ;

Borges, L. E. P. ;

Mattos, L. V. ;

Noronha, F. B. .

CATALYSIS TODAY, 2008, 133 (755-761) :755-761

[28] Production of CO-free H2 from formic acid. A comparative study of the catalytic behavior of Pt metals on a carbon support [J].

Solymosi, F. ;

Koos, A. ;

Liliom, N. ;

Ugrai, I. .

JOURNAL OF CATALYSIS, 2011, 279 (01) :213-219

[29] Adsorption/Desorption Behavior of Ethanol Steam Reforming Reactants and Intermediates over Supported Cobalt Catalysts [J].

Song, Hua ;

Bao, Xiaoguang ;

Hadad, Christopher M. ;

Ozkan, Umit S. .

CATALYSIS LETTERS, 2011, 141 (01) :43-54

[30] Combined DFT, Microkinetic, and Experimental Study of Ethanol Steam Reforming on Pt [J].

Sutton, Jonathan E. ;

Panagiotopouou, Paraskevi ;

Veryldos, Xenophon E. ;

Vlachos, Dionisios G. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (09) :4691-4706

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