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High Selectivity to Aromatics by a Mg and Na Co-modified Catalyst in Direct Conversion of Syngas

机译:用Mg和Na共改性催化剂在合成气的直接转化中对芳烃的选择性高

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The demand for aromatics, especially benzene, toluene, and xylene, has been increased in recent years as the crucial feedstocks of coatings and pharmaceutical industry. In this work, a modified Fischer–Tropsch synthesis (FTS) catalyst FeNaMg was fabricated via a sol-precipitation method and integrated with an HZSM-5 aromatization catalyst for the aromatics synthesis from syngas by a one-step process. Syngas was first converted to lower olefins as intermediates on the active component of the FeNaMg catalyst followed by aromatization on zeolite. Different characterization approaches, such as BET, XRD, XPS, hydrogen temperature-programmed reduction, temperature-programmed desorption of CO, TG, and SEM, revealed that Mg efficiently optimized physicochemical properties of the Fe-based catalyst by generating a MgFe_(2)O_(4) spinel structure. Further investigation demonstrated that the MgFe_(2)O_(4) spinel structure could increase the syngas adsorption area, facilitating the reduction and carburization of the Fe phase, while Mg decreased CO_(2) selectivity (31.26 to21%) by restraining the water–gas shift reaction and improved the utilization efficiency of carbon. At the same time, alkali metal Na changed the surface electronic environment of the FTS catalyst to enhance CO adsorption as an electronic promoter, which suppressed methane formation by restraining over hydrogenation. Therefore, the synergism that existed between Mg and Na during the reaction escalated the CO conversion and aromatics selectivity to 96.19 and 51.38%, respectively.
机译:近年来,对芳烃,尤其是苯,甲苯和二甲苯的需求,作为涂料和制药行业的关键原料。在这项工作中,通过溶胶沉淀法制造改性的Fischer-Tropsch合成(FTS)催化剂FENAMG,并通过一步法与合成气合成的HZSM-5芳族化催化剂集成。首先将合成气转化为下烯烃作为FENAMG催化剂的活性组分的中间体,然后在沸石上芳香化。不同的表征方法,例如BET,XRD,XPS,氢气温度编程,CO,TG和SEM的温度编程解吸,显示MG通过产生MGFE_(2)有效地优化了Fe基催化剂的物理化学性质O_(4)尖晶石结构。进一步的研究表明,MgFe_(2)O_(4)尖晶石结构可以增加合成气吸附区域,促进Fe相的减少和渗碳,而Mg通过限制水(31.26至21%)降低CO_(2)选择性 - 煤气变换反应和提高碳的利用效率。同时,碱金属NA改变了FTS催化剂的表面电子环境,以增强CO吸附作为电子促进剂,通过限制氢化来抑制甲烷的形成。因此,在反应过程中,在Mg和Na之间存在的协同作用升级为96.19和51.38%的CO转化和芳烃选择性。

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