Wang Chao, Zhao Xingling, Hu Min, Qi Guodong, Wang Qiang, Li Shenhui, Xu Jun, Deng Feng
National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, 430071, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2021 Oct 25;60(44):23630-23634. doi: 10.1002/anie.202111111. Epub 2021 Oct 1.
Propane aromatization on metal-modified zeolites provides a promising route to produce valuable chemicals such as benzene, toluene and xylene via non-petroleum feedstocks. The mechanistic understanding of propane conversion to aromatics is still challenging due to the complexity of the aromatization process. Herein, by using solid-state NMR spectroscopy and GC-MS, it is shown that cyclopentenyl cations are formed as active intermediates during propane aromatization on Ga/ZSM-5 zeolite. Autocatalysis of propane to aromatics is identified in the induction period. The cyclopentenyl cations serve as key hydrocarbon pool species to co-catalyze propane conversion and promote aromatics formation, revealing a dominant hydrocarbon pool process in propane aromatization.
金属改性沸石上的丙烷芳构化提供了一条通过非石油原料生产苯、甲苯和二甲苯等有价值化学品的有前景的途径。由于芳构化过程的复杂性,对丙烷转化为芳烃的机理理解仍然具有挑战性。在此,通过使用固态核磁共振光谱和气相色谱 - 质谱联用技术表明,在Ga/ZSM - 5沸石上的丙烷芳构化过程中,环戊烯基阳离子作为活性中间体形成。在诱导期确定了丙烷到芳烃的自催化作用。环戊烯基阳离子作为关键的烃池物种共同催化丙烷转化并促进芳烃形成,揭示了丙烷芳构化中主要的烃池过程。