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Fischer–Tropsch Synthesis: ZIF-8@ZIF-67-Derived Cobalt Nanoparticle-Embedded Nanocage Catalysts
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-06-10 , DOI: 10.1021/acs.iecr.0c00971
Baozhong Lü 1, 2, 3, 4 , Weijie Qi 1, 3 , Mingsheng Luo 1, 3 , Qinglong Liu 1, 3 , Lin Guo 4
Affiliation  

The preparation of highly active and stable catalysts for syngas conversion is a major challenge for Fischer–Tropsch synthesis (FTS). Herein, we report a strategy to prepare a highly dispersed Co-embedded porous carbon nanocage (CoPCN) structure derived from a core–shell metal–organic framework (MOF) ZIF-8@ZIF-67 precursor. High Co loading (over wt 30%) is achieved while maintaining an optimal dispersion and particle size of the active Co phase when a ZIF-8@ZIF-67 is pyrolyzed at 920 °C. Besides, the porous channels and hollow structures of the CoPCN strengthen the diffusion of reactants and the hydrocarbon product, enhancing the C5+ selectivity and CO conversion. The CoPCN shows high stability in FTS with a CO conversion of 18.3%, 80.2% selectivity for long-chain hydrocarbons (C5+), and 8.9% selectivity for short-chain hydrocarbons (C2–C4) after 100 h time on stream. Compared with other MOF-derived FTS catalysts, CoPCN-920 can achieve higher C5+ selectivity at a lower reaction temperature. The present work uncovers the relationship between the porous structure and catalytic performance, providing an efficient method to prepare promising materials for enhanced FTS stability, activity, and selectivity.

中文翻译:

费-托合成:ZIF-8 @ ZIF-67衍生的钴纳米颗粒嵌入式纳米笼催化剂

制备用于合成气转化的高活性和稳定的催化剂是费托合成(FTS)的主要挑战。在这里,我们报告了一种策略,该策略准备了一种从核-壳金属-有机骨架(MOF)ZIF-8 @ ZIF-67前体衍生的高度分散的共嵌入多孔碳纳米笼(CoPCN)结构。当在920°C下热解ZIF-8 @ ZIF-67时,可实现高Co负载量(超过30%wt),同时保持活性Co相的最佳分散度和粒径。此外,CoPCN的多孔通道和中空结构增强了反应物和烃产物的扩散,提高了C 5+的选择性和CO的转化率。CoPCN在FTS中显示出高稳定性,CO转化率为18.3%,对长链烃(C 5+),在运行100小时后,对短链碳氢化合物(C 2 –C 4)的选择性为8.9%。与其他MOF衍生的FTS催化剂相比,CoPCN-920在较低的反应温度下可以实现更高的C 5+选择性。本工作揭示了多孔结构与催化性能之间的关系,为制备有望用于增强FTS稳定性,活性和选择性的材料提供了一种有效的方法。
更新日期:2020-06-10
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