Intrinsic properties of active sites for hydrogen production from alcohols without coke formation

摘要/Abstract

摘要： The detailed reaction pathway and coke formation mechanism over Pt/metal oxide nanoparticles during the steam reforming of ethanol (SRE) at 300 ℃ were studied. The catalysts were prepared by incipient wetness impregnation method and were characterized with CO pulse chemisorption, BET surface measurement, oxygen adsorption, ethanol-TPD, NH₃-TPD, and TPO. The SRE activity of the catalysts with steam/ethanol molar ratio of 3/1 was tested using a continuous fixed-bed reactor. Strong interaction between Pt and supports causes lower H₂ production temperatures and no C₂H₄ formation, while weak interaction leads to C₂H₄ formation and strong bonded CO on Pt particles during ethanol-TPD. H₂ production over Pt-based catalysts is mainly resulted from the decomposition and dehydrogenation of ethanol, and decarbonylation of acetaldehyde. Meanwhile, coke can be formed from acetaldehyde, acetone, C₂H₄ and CO. However, when the interaction between Pt and supports is weak, more coke is formed especially from acetone, C₂H₄ and CO. When the interaction is strong, no coke formation is observed due to high oxygen storage capacity of the catalyst.

关键词: active sites, hydrogen, alcohols, coke formation, Pt, interaction

Abstract: The detailed reaction pathway and coke formation mechanism over Pt/metal oxide nanoparticles during the steam reforming of ethanol (SRE) at 300 ℃ were studied. The catalysts were prepared by incipient wetness impregnation method and were characterized with CO pulse chemisorption, BET surface measurement, oxygen adsorption, ethanol-TPD, NH₃-TPD, and TPO. The SRE activity of the catalysts with steam/ethanol molar ratio of 3/1 was tested using a continuous fixed-bed reactor. Strong interaction between Pt and supports causes lower H₂ production temperatures and no C₂H₄ formation, while weak interaction leads to C₂H₄ formation and strong bonded CO on Pt particles during ethanol-TPD. H₂ production over Pt-based catalysts is mainly resulted from the decomposition and dehydrogenation of ethanol, and decarbonylation of acetaldehyde. Meanwhile, coke can be formed from acetaldehyde, acetone, C₂H₄ and CO. However, when the interaction between Pt and supports is weak, more coke is formed especially from acetone, C₂H₄ and CO. When the interaction is strong, no coke formation is observed due to high oxygen storage capacity of the catalyst.

Key words: active sites, hydrogen, alcohols, coke formation, Pt, interaction

Zhong He, Xianqin Wang. Intrinsic properties of active sites for hydrogen production from alcohols without coke formation[J]. 能源化学(英文), 2013, 22(3): 436-445.

Zhong He, Xianqin Wang. Intrinsic properties of active sites for hydrogen production from alcohols without coke formation[J]. Journal of Energy Chemistry, 2013, 22(3): 436-445.

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