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作 者:裴彦鹏[1,2] 丁云杰[1,3] 朱何俊[1] 杜虹[1,2]
机构地区:[1]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 [2]中国科学院大学,北京100049 [3]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
出 处:《催化学报》2015年第3期355-361,共7页
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Si O2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,Si O2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Si O2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Si O2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.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 phy‐sisorption techniques were all employed to assess the catalyst. Although the addition of SiO2 de‐creased the reducibility of the Co component, Co dispersion was significantly increased and its ag‐gregation 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 capa‐ble of facilitating CO insertion.
关 键 词:钴催化剂 高碳醇 二氧化硅助剂 费托合成 碳化钴
分 类 号:TQ529.2[化学工程—煤化学工程] O643.36[理学—物理化学]
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