Fischer-Tropsch synthesis: Anchoring of cobalt particles in phosphorus modified cobalt/silica catalysts

被引:19
|
作者
Gnanamani, Muthu Kumaran [1 ]
Jacobs, Gary [1 ]
Pendyala, Venkat Ramana Rao [1 ]
Graham, Uschi M. [1 ]
Hopps, Shelley D. [1 ]
Thomas, Gerald A. [1 ]
Shafer, Wilson D. [1 ]
Sparks, Dennis E. [1 ]
Xiao, Qunfeng [2 ]
Hu, Yongfeng [2 ]
Davis, Burtron H. [1 ]
机构
[1] Univ Kentucky, Ctr Appl Energy Res, 2540 Res Pk Dr, Lexington, KY 40511 USA
[2] Canadian Light Source Inc, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada
基金
加拿大健康研究院; 加拿大创新基金会; 加拿大自然科学与工程研究理事会;
关键词
Fischer-Tropsch synthesis; Cobalt; Silica; Phosphorus; Promoter; EXAFS/XANES; IN-SITU EXAFS; L-III EDGES; CO/AL2O3; CATALYSTS; BIMETALLIC CATALYSTS; REDUCTION PROPERTY; CARBON DEPOSITION; CO-CATALYSTS; ALUMINA; SUPPORT; DEACTIVATION;
D O I
10.1016/j.apcata.2016.05.024
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
The effect of phosphorus addition on silica-supported cobalt catalyst was investigated for Fischer-Tropsch synthesis (FTS). As shown by STEM images and chemisorption, the addition of phosphorus to cobalt of up to 1 wt% increased the dispersion of cobalt. Further addition of phosphorus (e.g., 3 and 5 wt.%), as demonstrated by TPR, pulse reoxidation, and XANES, significantly hindered the reduction of cobalt oxides. The cobalt FTS catalysts containing 0.5 and 1.0 wt% P exhibited greater stability in comparison with undoped and 3.0 wt% P containing cobalt catalysts. Analysis of XANES spectra at the P and Co K-edges, along with DRIFTS results of H-2-activated cobalt catalysts, suggest that cobalt particles interact with PO43- ions, indicating a role played by P in anchoring Co particles to the support, thus hindering the cobalt sintering rate. The initial selectivity to methane was slightly higher for 0.5%P-20%Co/SiO2 and 1.0%P-20%Co/SiO2 catalysts compared to the undoped catalyst, but at longer times differences were small. At higher loadings of P (3 wt.%), FT activity and selectivity were adversely and irreversibly affected. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:146 / 158
页数:13
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