Influence of oxygen-containing surface groups on the activity and selectivity of carbon nanofiber-supported ruthenium catalysts in the hydrogenation of cinnamaldehyde

被引:216
作者
Toebes, ML
Prinsloo, FF
Bitter, JH
van Dillen, AJ
de Jong, KP
机构
[1] Univ Utrecht, Dept Inorgan Chem & Catalysis, Debye Inst, NL-3508 TB Utrecht, Netherlands
[2] Sasol Technol R&D, ZA-9570 Sasolburg, South Africa
关键词
carbon nanofibers; CNF; ruthenium catalyst; oxygen-containing surface groups; cinnamaldehyde hydrogenation; homogeneous deposition precipitation; metal-support interaction;
D O I
10.1016/S0021-9517(02)00081-7
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
Carbon-nanofiber-supported ruthenium catalysts were employed to study the influence of oxygen-containing surface groups on catalytic performance in the liquid-phase hydrogenation of cinnamaldehyde. The carbon nanofibers were oxidized to introduce oxygen-containing groups and the metal precursor was applied using homogeneous deposition precipitation. After reduction the catalysts were heat-treated in nitrogen at different temperatures to tune the number of surface oxygen functional groups. TEM and chemisorption studies showed the presence of a narrow and stable particle-size distribution (1-2 nm) even after heat treatment at 973 K. The overall specific activity increased by a factor of 22 after treatment at 973 K, which is related to the decreasing number of oxygen-containing groups. The cinnamyl alcohol selectivity decreases from 48 to 8% due to enhanced rate of hydrocinnamaldehyde production with increasing heat treatment. This unambiguously demonstrates the metal-support interaction, which involves support surface-oxygen functionalities that affect the metal activity and selectivity. The precise nature of this interaction has yet to be elucidated. (C) 2003 Elsevier Science (USA). All rights reserved.
引用
收藏
页码:78 / 87
页数:10
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