期刊
APPLIED CATALYSIS A-GENERAL
卷 502, 期 -, 页码 71-77出版社
ELSEVIER
DOI: 10.1016/j.apcata.2015.05.037
关键词
Isobutene; Supercritical fluids; Metal-free catalysis; Carbon catalysts; Oxidative dehydrogenation
资金
- Spanish Ministerio de Economia y Competitividad [CTQ2012-30909]
- Anticipios Fondos Feder
- FCT - Fundacao para a Ciencia e a Tecnologia [UID/EQU/50020/2013]
- FEDER [UID/EQU/50020/2013, NORTE-07-0162-FEDER-000050, NORTE-07-0124-FEDER-000015]
- QREN under Programe COMPETE [NORTE-07-0162-FEDER-000050, NORTE-07-0124-FEDER-000015]
- ON2 under Programe COMPETE [NORTE-07-0162-FEDER-000050, NORTE-07-0124-FEDER-000015]
- FCT under Programe COMPETE [SFRH/BPD/97689/2013]
Modifications that supercritical fluids promote in the surface chemistry of carbon materials are scarcely investigated. Due to this lack of knowledge, carbon materials exposed to supercritical fluids have not been tested in any catalytic application. Here, we present the oxidative dehydrogenation of isobutane catalyzed by an activated carbon fiber cloth previously exposed to supercritical carbon dioxide, supercritical water and nitric acid. The role of carbonyl quinone groups as active sites is confirmed by their direct correlation with catalytic activity. The ability of the active sites to produce isobutene is hindered by the presence of acidic groups. Supercritical treatments develop microporosity, while removing acidic oxygen surface groups and incorporating carbonyl quinone groups, so they are appropriate methods to develop efficient carbon catalysts for this reaction. Coke deposits formed during reaction modify the surface chemistry and porosity of the catalysts. Samples presenting high surface areas are deactivated by coke deposition more slowly. Thanks to it, fibers exposed to supercritical water showed the best performance. (C) 2015 Elsevier B.V. All rights reserved.
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