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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.
Coke-induced catalyst deactivation draws increasing concerns in industrially catalytic processes. Here the authors provide a strategy integrating advanced mass spectroscopy and isotope labeling to uncover a cage-passing molecular route of coking species in molecular sieve catalysts.
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1 Chinese Academy of Sciences, National Engineering Laboratory for Methanol to Olefins, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Dalian, PR China (GRID:grid.9227.e) (ISNI:0000000119573309); University of Chinese Academy of Sciences, Beijing, PR China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419)
2 Chinese Academy of Sciences, National Engineering Laboratory for Methanol to Olefins, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Dalian, PR China (GRID:grid.9227.e) (ISNI:0000000119573309)
3 Chinese Academy of Sciences, National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Wuhan, PR China (GRID:grid.9227.e) (ISNI:0000000119573309)
4 Chinese Academy of Sciences, National Engineering Laboratory for Methanol to Olefins, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Dalian, PR China (GRID:grid.9227.e) (ISNI:0000000119573309); Chinese Academy of Sciences, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian, PR China (GRID:grid.9227.e) (ISNI:0000000119573309)