Selectivity modulation in Fischer-Tropsch synthesis through reducibility control of cobalt-species containing HMS framework

IF 5.2 2区 化学 Q1 CHEMISTRY, APPLIED Catalysis Today Pub Date : 2024-10-23 DOI:10.1016/j.cattod.2024.115110
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Abstract

Here reports the modulation of selectivity in Fischer-Tropsch synthesis through the control of cobalt reducibility within a hexagonal mesoporous silica (HMS) framework. Cobalt loading, varied from 3 % to 12.5 wt%, generated different surface and bulk cobalt species that interact variably with the support, significantly influencing their reducibility and the resultant catalytic behavior. This variation significantly affected the reducibility of the cobalt species, influencing on the catalytic behavior. The control of reducibility and stability of Co species is contingent on the cobalt loading. Higher cobalt content enhances the reducibility of Co species, shifting product selectivity from long-chain hydrocarbons to lighter olefins and oxygenates. At a TOS of 4 h, the active phase predominantly involves metallic Co species, while CO2 and oxygenates formation is closely linked to the pair Co0-Co2+ active phase. After a TOS of 120 h, samples with higher cobalt content (6.1–15.8 % wt.) exhibited notable deactivation and changes in selectivity and hydrocarbon distribution. These changes were associated with the formation of a Co2C phase, which inhibits methane formation and chain growth while enhancing the production of lower olefins and oxygenates through a synergistic interaction at the Co0 and Co2C interface, also improves the WGS reaction, thereby increasing CO2 selectivity.
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通过控制含钴种 HMS 框架的还原性调节费托合成中的选择性
本文报告了通过控制六方介孔二氧化硅(HMS)框架内的钴还原性来调节费托合成中的选择性。钴的负载量从 3% 到 12.5 wt% 不等,产生了不同的表面和块体钴物种,这些钴物种与支持物的相互作用各不相同,极大地影响了它们的还原性和由此产生的催化行为。这种变化极大地影响了钴物种的还原性,从而影响了催化行为。钴物种的还原性和稳定性取决于钴的负载量。钴含量越高,钴物种的还原性越强,产品选择性从长链烃类转向较轻的烯烃和含氧化合物。在 4 小时的总反应时间内,活性相主要涉及金属 Co 物种,而 CO2 和含氧化合物的形成则与一对 Co0-Co2+ 活性相密切相关。在 120 小时的 TOS 之后,钴含量较高的样品(6.1-15.8% wt.)表现出明显的失活以及选择性和碳氢化合物分布的变化。这些变化与 Co2C 相的形成有关,Co2C 相通过 Co0 和 Co2C 界面的协同作用,抑制了甲烷的形成和链增长,同时提高了低级烯烃和含氧化合物的产量,还改善了 WGS 反应,从而提高了二氧化碳的选择性。
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来源期刊
Catalysis Today
Catalysis Today 化学-工程:化工
CiteScore
11.50
自引率
3.80%
发文量
573
审稿时长
2.9 months
期刊介绍: Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.
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