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Direct aromatization of CO2 via combined CO2 hydrogenation and zeolite-based acid catalysis
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-01-20 , DOI: 10.1016/j.jcou.2020.101405
Iman Nezam , Wei Zhou , Gabriel S. Gusmão , Matthew J. Realff , Ye Wang , Andrew J. Medford , Christopher W. Jones

Aromatics, including benzene, toluene, and xylenes (BTX), are essential chemical building blocks and are widely used as solvents, fuel additives, and polymers. With the recent development in CO2 capture technologies and the progress made in producing H2 using renewable energy, direct hydrogenation of CO2 to aromatics via heterogeneous catalysis has emerged as a promising pathway to accomplish the production of aromatics with simultaneous utilization of waste CO2. In this review, we focus on recent advances in the nascent field of direct CO2 aromatization, whereby tandem catalysts composed of CO2 hydrogenation and aromatization functionalities are designed and deployed. We review two categories of tandem catalysts: catalysts integrating Fe-based/H-ZSM-5 components following RWGS (reverse water-gas shift of CO2 to CO)-FT (Fischer-Tropsch synthesis of lower olefins)-aromatization pathways, and catalysts combining metal oxide/H-ZSM-5 domains following CO2 to methanol-aromatization pathways. The key parameters that determine the catalytic performance, such as the composition and structure of the Fe-based or metal oxide-based CO2 conversion catalysts, the properties of H-ZSM-5, and the synergy between the two components, are analyzed to provide insights for the design of efficient tandem catalysts for CO2 aromatization. In parallel, thermodynamic analyses, mechanistic studies, and density functional theory (DFT) computations for the relevant reaction routes and pathways are discussed to offer improved understanding of CO2 activation, reaction intermediates, and product formation. Finally, the challenges and prospects for these tandem reactions are addressed to provide suggested paths forward for future research.



中文翻译:

通过将CO 2加氢和基于沸石的酸催化相结合直接将CO 2芳香化

芳香族化合物,包括苯,甲苯和二甲苯(BTX),是必不可少的化学结构单元,被广泛用作溶剂,燃料添加剂和聚合物。随着CO 2捕集技术的最新发展以及利用可再生能源生产H 2的进展,通过多相催化将CO 2直接加氢成芳烃已成为一种有前景的途径,可以同时利用废CO 2完成芳烃的生产。。在这篇综述中,我们关注于直接CO 2芳构化新兴领域的最新进展,其中由CO 2组成的串联催化剂设计并部署了氢化和芳构化功能。我们回顾了两类串联催化剂:RWGS(CO 2向CO的反水煤气转化为CO)-FT(低级烯烃的费-托合成)-芳构化路径后结合铁基/ H-ZSM-5组分的催化剂;以及催化剂将CO 2之后的金属氧化物/ H-ZSM-5结构域结合到甲醇芳构化路径中。分析了决定催化性能的关键参数,例如铁基或金属氧化物基CO 2转化催化剂的组成和结构,H-ZSM-5的性质以及两种组分之间的协同作用,为设计高效的CO 2串联催化剂提供见解芳香化。同时,对相关反应路线和途径的热力学分析,机理研究和密度泛函理论(DFT)计算进行了讨论,以提高对CO 2活化,反应中间体和产物形成的理解。最后,解决了这些串联反应的挑战和前景,为今后的研究提供了建议的途径。

更新日期:2021-01-20
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