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铁对3D打印不锈钢微通道微反应器中用于费托合成的钴基SiOAlO混合载体催化剂的影响。

Effect of Fe on Co-Based SiOAlO Mixed Support Catalyst for Fischer-Tropsch Synthesis in 3D-Printed SS Microchannel Microreactor.

作者信息

Arslan Meric, Bepari Sujoy, Shajahan Juvairia, Hassan Saif, Kuila Debasish

机构信息

Department of Applied Science and Technology, North Carolina Agricultural and Technical State University, Greensboro, NC 27411, USA.

Department of Chemistry, North Carolina Agricultural and Technical State University, Greensboro, NC 27411, USA.

出版信息

Molecules. 2025 Aug 25;30(17):3486. doi: 10.3390/molecules30173486.

Abstract

This research explores the effect of a composite support of SiO and AlO with Fe and Co incorporated as catalysts for Fischer-Tropsch synthesis (FTS) using a 3D-printed stainless steel (SS) microchannel microreactor. Two mesoporous catalysts, FeCo/SiOAlO and Co/SiOAlO, were synthesized via a one-pot (OP) method and extensively characterized using N physisorption, XRD, SEM, TEM, H-TPR, TGA-DSC, FTIR, and XPS. H-TPR results revealed that the synthesis method significantly affected the reducibility of metal oxides, thereby influencing the formation of active FTS sites. SEM-EDS and TEM further revealed a well-defined hexagonal matrix with a porous surface morphology and uniform metal ion distribution. FTS reactions, carried out in the 200-350 °C temperature range at 20 bar with a H/CO molar ratio of 2:1, exhibited the highest activity for FeCo/SiOAlO, with up to 80% CO conversion. Long-term stability was evaluated by monitoring the catalyst performance for 30 h on stream at 320 °C under identical reaction conditions. The catalyst was initially active for the methanation reaction for up to 15 h, after which the selectivity for CH declined. Correspondingly, the C selectivity increased after 15 h of time-on-stream, indicating a shift in the product distribution toward longer-chain hydrocarbons. This trend suggests that the catalyst undergoes gradual activation or restructuring under reaction conditions, which enhances chain growth over time. The increase in C products may be attributed to the stabilization of the active sites and suppression of methane or light hydrocarbon formation.

摘要

本研究探索了采用3D打印不锈钢微通道微反应器,以负载铁和钴的SiO₂和Al₂O₃复合载体作为费托合成(FTS)催化剂的效果。通过一锅法合成了两种介孔催化剂FeCo/SiO₂Al₂O₃和Co/SiO₂Al₂O₃,并使用N₂物理吸附、XRD、SEM、TEM、H₂-TPR、TGA-DSC、FTIR和XPS对其进行了广泛表征。H₂-TPR结果表明,合成方法对金属氧化物的还原性有显著影响,从而影响活性FTS位点的形成。SEM-EDS和TEM进一步揭示了具有明确六边形结构、多孔表面形态和均匀金属离子分布的结构。在20 bar、H₂/CO摩尔比为2:1的条件下,于200-350 °C温度范围内进行的FTS反应中,FeCo/SiO₂Al₂O₃表现出最高活性,CO转化率高达80%。通过在相同反应条件下320 °C连续运行30 h监测催化剂性能来评估长期稳定性。催化剂最初对甲烷化反应具有活性,长达15 h,之后CH₄选择性下降。相应地,在运行15 h后,C₅⁺选择性增加,表明产物分布向长链烃类转移。这种趋势表明,催化剂在反应条件下会逐渐活化或重构,随着时间的推移促进链增长。C₅⁺产物的增加可能归因于活性位点的稳定以及甲烷或轻质烃类生成的抑制。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/441d/12430590/6078126d51cb/molecules-30-03486-g001.jpg

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