Methanol Steam Reforming over Indium-Promoted Pt/Al2O3 Catalyst: Nature of the Active Surface

被引:35
作者
Barbosa, Roland L. [1 ]
Papaefthimiou, Vasiliki [1 ]
Law, Yeuk T. [1 ]
Teschner, Detre [2 ]
Haevecker, Michael [2 ,4 ]
Knop-Gericke, Axel [2 ]
Zapf, Ralf [3 ]
Kolb, Gunther [3 ]
Schloegl, Robert [2 ]
Zafeiratos, Spyridon [1 ]
机构
[1] ICPEES, UMR Strasbourg 7515, F-67087 Strasbourg 2, France
[2] Fritz Haber Inst MPG, D-14195 Berlin, Dahlem, Germany
[3] Inst Mikrotech Mainz GmbH IMM, D-55129 Mainz, Germany
[4] Helmholtz Zentrum Berlin BESSY II, D-12489 Berlin, Germany
关键词
WATER-GAS SHIFT; HYDROGEN-PRODUCTION; OXIDATION-STATE; PLATINUM; ADSORPTION; REDUCTION; NANOPARTICLES; ALUMINUM; ALLOYS; OXIDES;
D O I
10.1021/jp309401q
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
The surface state of the Pt/In2O3/Al2O3 catalyst coated onto a microchannel stainless steel reactor was investigated under working conditions using synchrotron-based ambient pressure photoelectron (APPES) and X-ray absorption near-edge structure (XANES) spectroscopies, combined with online mass spectrometry. The surface of the fresh catalyst consists of metallic Pt, In2O3, and Al2O3. Reduction under 0.2 mbar of H-2 at 250 degrees C leads to surface enhancement of Pt and partial reduction of In2O3, while Al2O3 remains unchanged. Reoxidation in O-2 atmosphere stimulates surface segregation of In2O3 over Pt, accompanied by partial oxidation of Pt to PtOx. Based on these results a dynamic, gas-phase-dependent surface state is demonstrated. Under methanol steam reforming conditions, the surface state rapidly adapts under the reaction stream regardless of the pretreatment. However, correlation of gas phase with spectroscopic results under working conditions pointed out the beneficial effect of surface indium to reduce the CO selectivity. Finally, evidence of a distorted symmetry of Al sites on Pt/In2O3/Al2O3 catalyst compared to that of gamma-Al2O3 is given. The findings obtained in the present study are of fundamental significance in understanding the relation between the surface state and the catalytic performance of a functional methanol reforming catalyst.
引用
收藏
页码:6143 / 6150
页数:8
相关论文
共 50 条
[21]   Production of hydrogen by steam reforming of methanol on CeO2 promoted Cu/Al2O3 catalysts [J].
Zhang, XR ;
Shi, PF .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 194 (1-2) :99-105
[22]   Hydrogen production from low-temperature methanol steam reforming over silver-promoted CuO/ZnO/Ag/Al2O3 Catalyst [J].
Zhang, Saibei ;
Qu, Xiaohan ;
Lv, Hui ;
Mao, Jingbo ;
Zhou, Jinxia .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2024, 77 :1317-1326
[23]   Identification of active sites in CO oxidation over a Pd/Al2O3 catalyst [J].
Murata, Kazumasa ;
Eleeda, Eleen ;
Ohyama, Junya ;
Yamamoto, Yuta ;
Arai, Shigeo ;
Satsuma, Atsushi .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2019, 21 (33) :18128-18137
[24]   Methanol-steam reforming over a ZnO-Cr2O3/CeO2-ZrO2/Al2O3 catalyst [J].
Cao, Weiqiang ;
Chen, Guangwen ;
Li, Shulian ;
Yuan, Quan .
CHEMICAL ENGINEERING JOURNAL, 2006, 119 (2-3) :93-98
[25]   Effect of noble metal on oxidative steam reforming of methanol over CuO/ZnO/Al2O3 catalysts [J].
Chang, Cheng-Chun ;
Hsu, Che-Chuan ;
Chang, Ching-Tu ;
Chen, Yu-Pei ;
Liaw, Biing-Jye ;
Chen, Yin-Zu .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2012, 37 (15) :11176-11184
[26]   Optimization of hydrogen production by steam methane reforming over Y-promoted Ni/Al2O3 catalyst using response surface methodology [J].
Salahi, Fatemeh ;
Zarei-Jelyani, Fatemeh ;
Farsi, Mohammad ;
Rahimpour, Mohammad Reza .
JOURNAL OF THE ENERGY INSTITUTE, 2023, 108
[27]   Steam reforming of methanol over a Cu/ZnO/Al2O3 catalyst:: a kinetic analysis and strategies for suppression of CO formation [J].
Agrell, J ;
Birgersson, H ;
Boutonnet, M .
JOURNAL OF POWER SOURCES, 2002, 106 (1-2) :249-257
[28]   Modeling Open-Flow Steam Reforming of Methanol over Cu/ZnO/Al2O3 Catalyst in an Axisymmetric Reactor [J].
Pacheco, L. ;
Della-Valle, D. ;
Le Corre, O. ;
Habchi, C. ;
Lemenand, T. ;
Peerhossaini, H. .
JOURNAL OF APPLIED FLUID MECHANICS, 2015, 8 (01) :33-42
[29]   Parameter Study of Steam Methanol Reforming With Cu/ZnO/Al2O3 Catalyst in a Microchannel Reactor [J].
Lee, Chun-I ;
Shiu, Huan-Ruei ;
Chang, Wen-Chen ;
Tsau, Fang-Hei .
PROCEEDINGS OF THE 7TH INTERNATIONAL CONFERENCE ON FUEL CELL SCIENCE, ENGINEERING, AND TECHNOLOGY, 2009, :157-163
[30]   Insights into the effects of steam on propane dehydrogenation over a Pt/Al2O3 catalyst [J].
Shan, Yu-Ling ;
Zhu, Yi-An ;
Sui, Zhi-Jun ;
Chen, De ;
Zhou, Xing-Gui .
CATALYSIS SCIENCE & TECHNOLOGY, 2015, 5 (08) :3991-4000