Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (2): 257-269.

Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol

T. van Haasterecht, C. C. I. Ludding, K. P. de Jong, J. H. Bitter

Inorganic Chemistry and Catalysis, Utrecht University, PO Box 80083, 3508 TB Utrecht, The Netherlands

收稿日期:2012-12-06 修回日期:2013-02-25 出版日期:2013-03-20 发布日期:2013-04-04
通讯作者: J. H. Bitter
基金资助:
This work was supported by the Smart Mix Program of the Netherlands Ministry of Economic Affairs and the Netherlands Ministry of Education, Culture and Science.

Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol

T. van Haasterecht, C. C. I. Ludding, K. P. de Jong, J. H. Bitter

Inorganic Chemistry and Catalysis, Utrecht University, PO Box 80083, 3508 TB Utrecht, The Netherlands

Received:2012-12-06 Revised:2013-02-25 Online:2013-03-20 Published:2013-04-04
Supported by:
This work was supported by the Smart Mix Program of the Netherlands Ministry of Economic Affairs and the Netherlands Ministry of Education, Culture and Science.

摘要/Abstract

摘要： Nickel, cobalt, copper and platinum nanoparticles supported on carbon nano-fibers were evaluated with respect to their stability, catalytic activity and selectivity in the aqueous phase reforming of ethylene glycol (230 ℃, autogenous pressure, batch reactor). The initial surface-specific activities for ethylene glycol reforming were in a similar range but decreased in the order of Pt (15.5 h^-1)>Co(13.0 h^-1)>Ni(5.2 h^-1) while the Cu catalyst only showed low dehydrogenation activity. The hydrogen molar selectivity decreased in the order of Pt (53%)>Co(21%)>Ni (15%) as a result of the production of methane over the latter two catalysts. Over the Co catalyst acids were formed in the liquid phase while alcohols were formed over Ni and Pt. Due to the low pH of the reaction mixture, especially in the case of Co (as a result of the formed acids), significant cobalt leaching occurs which resulted in a rapid deactivation of this catalyst. Investigations of the spent catalysts with various techniques showed that metal particle growth is responsible for the deactivation of the Pt and Ni catalysts. In addition, coking might also contribute to the deactivation of the Ni catalyst.

关键词: carbon nano-fiber, catalyst deactivation, aqueous phase reforming, non-noble metal catalyst

Abstract: Nickel, cobalt, copper and platinum nanoparticles supported on carbon nano-fibers were evaluated with respect to their stability, catalytic activity and selectivity in the aqueous phase reforming of ethylene glycol (230 ℃, autogenous pressure, batch reactor). The initial surface-specific activities for ethylene glycol reforming were in a similar range but decreased in the order of Pt (15.5 h^-1)>Co(13.0 h^-1)>Ni(5.2 h^-1) while the Cu catalyst only showed low dehydrogenation activity. The hydrogen molar selectivity decreased in the order of Pt (53%)>Co(21%)>Ni (15%) as a result of the production of methane over the latter two catalysts. Over the Co catalyst acids were formed in the liquid phase while alcohols were formed over Ni and Pt. Due to the low pH of the reaction mixture, especially in the case of Co (as a result of the formed acids), significant cobalt leaching occurs which resulted in a rapid deactivation of this catalyst. Investigations of the spent catalysts with various techniques showed that metal particle growth is responsible for the deactivation of the Pt and Ni catalysts. In addition, coking might also contribute to the deactivation of the Ni catalyst.

Key words: carbon nano-fiber, catalyst deactivation, aqueous phase reforming, non-noble metal catalyst

T. van Haasterecht, C. C. I. Ludding, K. P. de Jong, J. H. Bitter. Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol[J]. 能源化学(英文), 2013, 22(2): 257-269.

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Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol

Stability and activity of carbon nanofiber-supported catalysts in the aqueous phase reforming of ethylene glycol

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