Effects of Co/SiO2 Particle Size on Fischer-Tropsch Synthesis: Study by TPD and DRIFTS

doi:10.6023/A15020133

Acta Chim. Sinica ›› 2015, Vol. 73 ›› Issue (7): 690-698.DOI: 10.6023/A15020133 Previous Articles Next Articles

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费托合成Co/SiO₂催化剂的粒子尺寸效应:TPD和DRIFTS的研究

邱成武^a,b, 吴宝山^a,c,d, 孟劭聪^a,b, 李永旺^a,c,d

a 中国科学院山西煤炭化学研究所煤转化国家重点实验室太原 030001;
b 中国科学院大学北京 100049;
c 煤炭间接液化国家工程实验室北京 101407;
d 中科合成油技术有限公司北京 101407

投稿日期:2015-02-15 发布日期:2015-07-07
通讯作者: 吴宝山 E-mail:wbs@sxicc.ac.cn
基金资助:
项目受国家自然科学基金(No. 21273261)资助.

Effects of Co/SiO₂ Particle Size on Fischer-Tropsch Synthesis: Study by TPD and DRIFTS

Qiu Chengwu^a,b, Wu Baoshan^a,c,d, Meng Shaocong^a,b, Li Yongwang^a,c,d

a State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001;
b University of Chinese Academy of Sciences, Beijing 100049;
c National Engineering Laboratory for Indirect Coal Liquefaction, Beijing 101407;
d Synfuels China Technology Co. LTD., Beijing 101407

Received:2015-02-15 Published:2015-07-07
Supported by:
Supporting information for this article is available free of charge via the Internet at http://sioc-journal.cn.Project supported by the National Natural Science Foundation of China (No. 21273261).

1. Effects of Co/SiO₂ Particle Size on Fischer-Tropsch Synthesis: Study by TPD and DRIFTS.PDF(210KB)

Abstract

The effects of cobalt particle size are still controversial for whether it influences Fischer-Tropsch synthesis (F-T synthesis) behavior intrinsically. In the F-T synthesis, a large number of different reaction pathways as well as multitude of products does result in many difficulties in the search for the intrinsic causes. The adsorption and dissociation of CO and H₂ is a key step for Fischer-Tropsch synthesis. So the effects are trying to be explained by means of exploring the relationship between the adsorbed behavior of CO and H₂ and cobalt particle size. In this work, four Co/SiO₂catalysts with different cobalt particle sizes, named 6, 8, 12, 19 nm, were prepared by incipient wetness impregnation using ethylene glycol (EG) and water mixture as a solvent. The catalysts were characterized by N₂ physisorption, X-Ray powder diffraction (XRD), transmission electron microscopy (TEM), temperature programmed desorption (TPD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and temperature programmed surface reaction (TPSR), and their Fischer-Tropsch reactivity were tested in a micro-fixed bed reactor. The F-T synthesis test showed that the catalysts with larger cobalt particle size had lower CO conversion, but their apparent Turnover Frequency (TOF) displayed a maximum for the catalyst with cobalt particle size of 8 nm. TPD and DRIFTS results indicated that both the adsorption and dissociation of CO were stronger on smaller cobalt particle, while some of the active sites could be blocked by carbon species on the surface, thus decreased the effective active sites. The adsorption of CO were weaker on larger cobalt particle and the formed C* species were easily desorbed, exhibiting higher CO*/Co_sratio on the surface. Therefore lower activity and higher CO₂ selectivity were observed. It is suggested that the catalyst with medium cobalt particle size can produce medium adsorbability of CO and proper amount of CO_ads (surface adsorbed CO) and C* species to balance suitable C/H ratio on the surface, exhibiting higher F-T activity and selectivity.

Key words: particle size, cobalt-based catalysts, F-T synthesis, TPD, DRIFTS

Cite this article

Qiu Chengwu, Wu Baoshan, Meng Shaocong, Li Yongwang. Effects of Co/SiO₂ Particle Size on Fischer-Tropsch Synthesis: Study by TPD and DRIFTS[J]. Acta Chim. Sinica, 2015, 73(7): 690-698.

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费托合成Co/SiO₂催化剂的粒子尺寸效应:TPD和DRIFTS的研究

Effects of Co/SiO₂ Particle Size on Fischer-Tropsch Synthesis: Study by TPD and DRIFTS

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费托合成Co/SiO2催化剂的粒子尺寸效应:TPD和DRIFTS的研究