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祝贺王超在Angew. Chem. Int. Ed杂志上发表文章

 日期:2021/11/18 12:19:24 浏览量:

Carbocations such as cyclic carbenium ions are important intermediates in the zeolite-catalyzed methanol-to-olefins (MTO) reaction. The MTO reaction propagates through a complex hydrocarbon pool process. Understanding the carbocation-involved hydrocarbon pool reaction on a molecular level still remains challenging. Here we show that electron-deficient cyclopentenyl cations stabilized in ZSM-5 zeolite are able to capture the alkanes, methanol, and olefins produced during MTO reaction via noncovalent interactions. Intermolecular spatial proximities/interactions are identified by using two-dimensional 13C–13C correlation solid-state NMR spectroscopy. Combined NMR experiments and theoretical analysis suggests that in addition to the dispersion and CH/π interactions, the multiple functional groups in the cyclopentenyl cations produce strong attractive force via cation-induced dipole, cation–dipole and cation–π interactions. These carbocation-induced noncovalent interactions modulate the product selectivity of hydrocarbon pool reaction.


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Link:https://onlinelibrary.wiley.com/doi/10.1002/anie.202112948


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