Ru添加对Co/SiO<sub>2</sub>费托合成催化剂性能的影响

邱成武; 吴宝山; 常强; 李永旺

Ru添加对Co/SiO₂费托合成催化剂性能的影响

邱成武^1,2,
吴宝山^1,3,4,,
常强^1,2,
李永旺^1,3,4

1.
中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001;
2.
中国科学院大学, 北京 100049;
3.
煤炭间接液化国家工程实验室, 北京 101407;
4.
中科合成油技术有限公司, 北京 101407

基金项目: 国家自然科学基金(21273261)资助项目

详细信息

通讯作者:
吴宝山,Tel:+86-10-69667779,E-mail:wbs@sxicc.ac.cn.

中图分类号: O643.36
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- 文章访问数: 375
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- 被引次数: 0
出版历程
- 收稿日期: 2015-03-10
- 修回日期: 2015-05-16
- 刊出日期: 2015-10-31

Effect of ruthenium addition on the performance of Co/SiO₂ catalyst for Fischer-Tropsch synthesis

QIU Cheng-wu^1,2,
WU Bao-shan^{1,3,4
,},
CHANG Qiang^1,2,
LI Yong-wang^1,3,4

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;
2.
University of Chinese Academy of Sciences, Beijing 100049, China;
3.
National Engineering Laboratory for Indirect Coal Liquefaction, Beijing 101407, China;
4.
Synfuels China Technology CO. LTD., Beijing 101407, China

Funds: The project was supported by the National Natural Science Foundation of China (21273261).

摘要

摘要: 用初湿含浸法制备了不同Ru添加量的Co/SiO₂模型催化剂,然后进行N₂物理吸附、XRD、H₂-TPD、DRIFTS等表征和微分固定床费托(F-T)反应评价。F-T反应结果表明,催化剂中添加Ru后,CO转化率显著提高,TOF值增大,CO₂和CH₄选择性降低,烯/烷比(O/P)降低。FT-IR表征说明,催化剂添加Ru后Co-O键的强度减弱,相对应的H₂-TPR也表明,催化剂的还原度得到显著提高。还原后的催化剂XRD结果进一步证实,加入Ru后,催化剂无钴氧化物被检出,并且当Ru添加量为0.5%(质量分数)时催化剂中金属钴主要以六方密堆(hcp)形式存在。CO-DRIFTS结果显示,Ru的加入使CO的吸收峰发生红移,即Ru促进了CO的解离。H₂-TPD结果则表明,随着Ru添加量的增加,催化剂表面CO_ads/Co_s和CO^*/Co_s增大,这是CH₄选择性降低的主要原因。
- Ru /
- 钴催化剂 /
- 表面吸附性 /
- F-T合成
Abstract: Three Co/SiO₂ catalysts doped with different amounts of Ru were prepared by incipient wetness impregnation. These catalysts were characterized by N₂ physisorption, XRD, H₂-TPD, DRIFTS, etc.; their catalytic performance in Fischer-Tropsch (F-T) synthesis was investigated in a micro fixed-bed reactor. The F-T reaction results showed that the Co/SiO₂ catalysts doped with Ru exhibit higher CO conversion, higher turnover frequency (TOF), lower selectivity to CO₂ and CH₄, as well as lower ratio of olefin to paraffin, in comparison with undoped Co/SiO₂. FT-IR spectra indicated that the Co-O bond in the as-prepared catalyst is weakened by the addition of Ru, which facilitates the reduction of the Co/SiO₂ catalysts; such results are also supported by the H₂-TPR profiles and XRD patterns of the reduced catalysts. The main cobalt phase in the reduced catalyst with 0.5% (by weight) of Ru is in a hexagonal close packing (hcp) structure. CO-DRIFTS results revealed that the peak of linearly adsorbed CO is red-shifted by the addition of Ru, suggesting an improvement on the dissociation of adsorbed CO. CO-TPD results showed that the ratio of CO_ads/Co_s and CO^*/Co_s on catalysts surface is increased by the addition of Ru, which may contribute to the decrease of the selectivity to CH₄ in F-T synthesis.
- Ru /
- cobalt catalyst /
- surface adsorption /
- F-T synthesis

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