Methanol steam reforming behavior of copper impregnated over CeO2-ZrO2 derived from a surfactant assisted coprecipitation route

被引:77
作者
Das, Dipak [1 ]
Llorca, Jordi [2 ]
Dominguez, Montserrat [2 ]
Colussi, Sara [3 ]
Trovarelli, Alessandro [3 ]
Gayen, Arup [1 ]
机构
[1] Jadavpur Univ, Dept Chem, Kolkata 700032, India
[2] Univ Politecn Cataluna, Inst Tecn Energet, Ctr Res Nanoengn, E-08028 Barcelona, Spain
[3] Univ Udine, Dipartimento Chim Fis & Ambiente, I-33100 Udine, Italy
关键词
Copper; Ceria-zirconia; Methanol steam reforming; Cu-sintering; Coking; Regeneration; OXYGEN STORAGE CAPACITY; HYDROGEN-PRODUCTION; CU/ZNO/AL2O3; CATALYSTS; SUPPORT MATERIAL; OXIDE CATALYSTS; ZIRCONIA; CERIA; DEACTIVATION; HYDROCARBONS; PERFORMANCE;
D O I
10.1016/j.ijhydene.2015.06.130
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
A series of ceria-zirconia solid solutions has been prepared by a surfactant assisted coprecipitation method. After impregnation of copper, their activities have been assessed for methanol steam reforming. The results indicate that the compositions with 10 and 15 at.% loading of copper on Ce0.6Zr0.4O2 exhibit maximum catalytic efficiency. Detailed structural analyses reveal high degree of copper dispersion on the ceria-zirconia matrix. In situ XPS studies confirm reduction of surface CuO species with concomitant lowering of Cu-surface atomic composition and increase of carbon. These evidences point to the formation of large aggregates of copper covered with coke that is suggested to be responsible for on stream activity loss. On regeneration, these aggregates break into a mixture of oxidized (Cu2+) and reduced (Cu-o and Cu+) copper species showing similar activity to the as prepared catalysts. In general, we have attributed catalytic activity to different proportions of copper components in the various forms of these catalysts. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:10463 / 10479
页数:17
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