活性炭负载的钴基催化剂催化费托合成反应一步合成C1-C18混合醇:二氧化硅助剂的作用

doi:10.1016/S1872-2067(14)60252-7

催化学报 ›› 2015, Vol. 36 ›› Issue (3): 355-361.DOI: 10.1016/S1872-2067(14)60252-7

活性炭负载的钴基催化剂催化费托合成反应一步合成C₁-C₁₈混合醇:二氧化硅助剂的作用

裴彦鹏^a,c, 丁云杰^a,b, 朱何俊^a, 杜虹^a,c

a 中国科学院大连化学物理研究所洁净能源国家实验室(筹), 辽宁大连116023;
b 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连116023;
c 中国科学院大学, 北京100049

收稿日期:2014-09-13 修回日期:2014-11-12 出版日期:2015-02-14 发布日期:2015-02-14
通讯作者: 丁云杰

One-step production of C₁-C₁₈ alcohols via Fischer-Tropsch reaction over activated carbon-supported cobalt catalysts: Promotional effect of modification by SiO₂

Yanpeng Pei^a,c, Yunjie Ding^a,b, Hejun Zhu^a, Hong Du^a,c

a Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
c University of Chinese Academy of Sciences, Beijing 100049, China

Received:2014-09-13 Revised:2014-11-12 Online:2015-02-14 Published:2015-02-14

摘要/Abstract

摘要：

采用费托合成反应以及X射线衍射、H₂程序升温还原、CO脉冲化学吸附和N₂物理吸附表征手段研究了SiO₂助剂对活性炭负载的钴基催化剂上生成C₁-C₁₈混合醇的影响. 结果表明, SiO₂的添加抑制了钴物种的还原, 但提高了钴物种的分散度, 同时抑制了金属钴颗粒在反应过程中的团聚, 从而显著提高了催化剂的活性. 适量SiO₂的添加促进了碳化钴的生成, 从而提高了总醇选择性. 重要的是, 通过SiO₂抑制钴物种的还原, 导致大量二价钴物种的生成, 从而有助于CO插入到碳链中间体中而使高碳醇容易生成.

关键词: 钴催化剂, 高碳醇, 二氧化硅助剂, 费托合成, 碳化钴

Abstract:

The promotional effect of SiO₂ on the catalytic synthesis of mixed C₁-C₁₈ alcohols from syngas using the Fischer-Tropsch reaction over activated carbon-supported cobalt catalysts was investigated. X-ray diffraction, H₂ temperature-programmed reduction, pulsed CO chemisorption and N₂ physisorption techniques were all employed to assess the catalyst. Although the addition of SiO₂ decreased the reducibility of the Co component, Co dispersion was significantly increased and its aggregation during reaction was inhibited, resulting in greatly enhanced reaction activity. Appropriate amounts of SiO₂ also promoted the formation of Co₂C, leading to an increased selectivity for C₁-C₁₈ alcohols. More importantly, the addition of SiO₂ favored the formation of higher molecular mass alcohols (C₆-C₁₈) by suppressing Co reduction, thus producing an abundance of Co(II) species capable of facilitating CO insertion.

Key words: Co catalyst, Higher alcohol, SiO₂ promoter, Fischer-Tropsch synthesis, Co₂C

裴彦鹏, 丁云杰, 朱何俊, 杜虹 . 活性炭负载的钴基催化剂催化费托合成反应一步合成C₁-C₁₈混合醇:二氧化硅助剂的作用[J]. 催化学报, 2015, 36(3): 355-361.

Yanpeng Pei, Yunjie Ding, Hejun Zhu, Hong Du. One-step production of C₁-C₁₈ alcohols via Fischer-Tropsch reaction over activated carbon-supported cobalt catalysts: Promotional effect of modification by SiO₂[J]. Chinese Journal of Catalysis, 2015, 36(3): 355-361.

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活性炭负载的钴基催化剂催化费托合成反应一步合成C₁-C₁₈混合醇:二氧化硅助剂的作用

One-step production of C₁-C₁₈ alcohols via Fischer-Tropsch reaction over activated carbon-supported cobalt catalysts: Promotional effect of modification by SiO₂

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