Comparative study of propane dehydrogenation over V-, Cr-, and Pt-based catalysts: Time on-stream behavior and origins of deactivation

被引:143
|
作者
Sokolov, Sergey [1 ]
Stoyanova, Mariana [1 ]
Rodemerck, Uwe [1 ]
Linke, David [1 ]
Kondratenko, Evgenii V. [1 ]
机构
[1] Univ Rostock, Leibniz Inst Katalyse eV, D-18059 Rostock, Germany
关键词
Propane; Dehydrogenation; Catalyst lifetime; Coke formation; In situ UV/Vis spectroscopy; SUPPORTED VANADIUM-OXIDE; OXIDATIVE DEHYDROGENATION; SELECTIVE CATALYSTS; N-BUTANE; OXYDEHYDROGENATION; SPECTROSCOPY; REACTIVITY; PLATINUM; ALKANES; SURFACE;
D O I
10.1016/j.jcat.2012.06.005
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
Catalytic performance of VOx/MCM-41 possessing highly dispersed VOx species in non-oxidative propane dehydrogenation (DH) was compared with that of industrially relevant CrOx/MCM-41 and Pt-Sn/Al2O3 over four DH (24 h on-stream) and oxidative regeneration cycles. The effect of reduction with H-2 on the catalysts DH properties was also investigated. VOx/MCM-41 in both oxidized and reduced form showed superior time on-stream stability in all DH cycles and its activity could be fully recovered by oxidative regeneration. In situ time-resolved UV/Vis spectroscopy and temperature-programmed oxidation of the used catalysts enabled us to elucidate the origins of the catalysts deactivation. In a single DH cycle, the formation of carbon deposits is the main reason for the deactivation. Activity loss of CrOx/MCM-41 and Pt-Sn/Al2O3 from cycle to cycle was caused by structural changes in the catalytically active metal/metal oxide species. In contrast to these two catalysts, the structure of active VOx species on MCM-41 was not changed during the DH/regeneration cycles, which is the reason for stable performance of the latter catalyst. (C) 2012 Elsevier Inc. All rights reserved.
引用
收藏
页码:67 / 75
页数:9
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