Structural characterization and catalytic performance of alkali (K) and metal (Co and Rh)-promoted MoS2 catalysts for higher alcohols synthesis

被引:31
作者
Surisetty, Venkateswara Rao [1 ]
Hu, Yongfeng [2 ]
Dalai, Ajay Kumar [1 ]
Kozinski, Janusz [3 ]
机构
[1] Univ Saskatchewan, Dept Chem Engn, Catalysis & Chem React Engn Labs, Saskatoon, SK S7N 5A9, Canada
[2] Canadian Light Source, Saskatoon, SK S7N 0X4, Canada
[3] York Univ, Fac Sci & Engn, Toronto, ON M3J 1P3, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
Higher alcohols synthesis; X-ray absorption near-edge structures; Alkali-promoted molybdenum catalyst; Multi-walled carbon nanotubes; Rh promotion; Co promotion; Trimetallic catalyst; CARBON NANOTUBES; L-EDGE; MOLYBDENUM CATALYSTS; XANES; HYDROGEN; SULFUR; OXIDES; H2S; DESULFURIZATION; BEHAVIOR;
D O I
10.1016/j.apcata.2010.11.006
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
A series of alkali and metal (Rh and Co) promoted MoS2 catalysts were prepared for the higher alcohols synthesis reaction. The effects of alkali and metal promoters on the performance and structure of molybdenum-sulfided catalysts were studied using the BET, X-ray diffraction (XRD), and X-ray absorption near edge structure (XANES) at the S K-edge and Mo L-3-edge. Alkali (K) promotion to trimetallic (Co-Rh-Mo) catalyst supported on multi-walled carbon nanotubes (MWCNTs) showed less CO conversion compared to that of the catalyst without K. The promotion of alkali reduces the hydrogenation ability of alkyl species to form alkanes and increases the active sites for the formation of alcohols, which is consistent with the observation of higher surface area and larger pore diameters in the K-promoted catalysts. XRD patterns showed that alkali-promoted catalysts were less crystalline compared to that of the catalyst not promoted with K. More oxidized S and Mo species were observed by XRD and XANES in the K-promoted catalysts, indicating the formation of more Mo oxide with the addition of K. thus increasing the active sites. The alkali-promoted trimetallic catalysts using two different supports, MWCNTs and active carbon (AC), showed very different catalytic performances. The activity of the AC-supported alkali-promoted trimetallic catalyst was lower than that supported on MWCNTs. More intense features corresponding to the oxidized S and Mo species were observed in both S K-edge and Mo L-3-edge spectra of the MWCNT-supported catalysts. Finally, formation of Co (Rh)-Mo-S species was evident in the XANES spectra of bimetallic and trimetallic alkali-promoted MoS2 catalysts, in agreement with their improved catalytic performance. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:166 / 172
页数:7
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