Kosinov Nikolay, Hensen Emiel J M
Laboratory of Inorganic Materials and Catalysis, Eindhoven University of Technology, P. O. Box 513, Eindhoven, MB, 5600, The Netherlands.
Adv Mater. 2020 Nov;32(44):e2002565. doi: 10.1002/adma.202002565. Epub 2020 Jul 12.
Non-oxidative dehydroaromatization is arguably the most promising process for the direct upgrading of cheap and abundant methane to liquid hydrocarbons. This reaction has not been commercialized yet because of the suboptimal activity and swift deactivation of benchmark Mo-zeolite catalysts. This progress report represents an elaboration on the recent developments in understanding of zeolite-based catalytic materials for high-temperature non-oxidative dehydroaromatization of methane. It is specifically focused on recent studies, relevant to the materials chemistry and elucidating i) the structure of active species in working catalysts; ii) the complex molecular pathways underlying the mechanism of selective conversion of methane to benzene; iii) structure, evolution and role of coke species; and iv) process intensification strategies to improve the deactivation resistance and overall performance of the catalysts. Finally, unsolved challenges in this field of research are outlined and an outlook is provided on promising directions toward improving the activity, stability, and selectivity of methane dehydroaromatization catalysts.
非氧化脱氢芳构化可以说是将廉价且丰富的甲烷直接升级为液态烃最具前景的工艺。由于基准钼沸石催化剂活性欠佳且迅速失活,该反应尚未实现商业化。本进展报告详细阐述了在理解用于甲烷高温非氧化脱氢芳构化的沸石基催化材料方面的最新进展。它特别关注了近期的研究,这些研究与材料化学相关,并阐明了:i) 工作催化剂中活性物种的结构;ii) 甲烷选择性转化为苯的机理背后复杂的分子途径;iii) 焦炭物种的结构、演变及作用;iv) 提高催化剂抗失活性和整体性能的过程强化策略。最后,概述了该研究领域尚未解决的挑战,并展望了提高甲烷脱氢芳构化催化剂活性、稳定性和选择性的有前景的方向。