Molecular elucidating of an unusual growth mechanism for polycyclic aromatic hydrocarbons in confined space

Nan Wang, Yuchun Zhi, Yingxu Wei (), Wenna Zhang, Zhiqiang Liu, Jindou Huang, Tantan Sun, Shutao Xu, Shanfan Lin, Yanli He, Anmin Zheng and Zhongmin Liu ()
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Nan Wang: Chinese Academy of Sciences
Yuchun Zhi: Chinese Academy of Sciences
Yingxu Wei: Chinese Academy of Sciences
Wenna Zhang: Chinese Academy of Sciences
Zhiqiang Liu: Chinese Academy of Sciences
Jindou Huang: Chinese Academy of Sciences
Tantan Sun: Chinese Academy of Sciences
Shutao Xu: Chinese Academy of Sciences
Shanfan Lin: Chinese Academy of Sciences
Yanli He: Chinese Academy of Sciences
Anmin Zheng: Chinese Academy of Sciences
Zhongmin Liu: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract Extension and clustering of polycyclic aromatic hydrocarbons (PAHs) are key mechanistic steps for coking and deactivation in catalysis reactions. However, no unambiguous mechanistic picture exists on molecule-resolved PAHs speciation and evolution, due to the immense experimental challenges in deciphering the complex PAHs structures. Herein, we report an effective strategy through integrating a high resolution MALDI FT-ICR mass spectrometry with isotope labeling technique. With this strategy, a complete route for aromatic hydrocarbon evolution is unveiled for SAPO-34-catalyzed, industrially relevant methanol-to-olefins (MTO) as a model reaction. Notable is the elucidation of an unusual, previously unrecognized mechanistic step: cage-passing growth forming cross-linked multi-core PAHs with graphene-like structure. This mechanistic concept proves general on other cage-based molecule sieves. This preliminary work would provide a versatile means to decipher the key mechanistic step of molecular mass growth for PAHs involved in catalysis and combustion chemistry.

Date: 2020
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DOI: 10.1038/s41467-020-14493-9

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