Molecular elucidating of an unusual growth mechanism for polycyclic aromatic hydrocarbons in confined space
Year: 2020
Type: article
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.
Source: Nature Communications
Authors: Nan Wang, Yuchun Zhi, Yingxu Wei, Wenna Zhang, Zhiqiang Liu, Zhiqiang Liu, Jindou Huang, Tantan Sun, Shutao Xu, Shanfan Lin, Yanli He, Anmin Zheng, Zhongmin Liu, Zhongmin Liu
Institutions: Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Collaborative Innovation Center of Chemistry for Energy Materials, University of Chinese Academy of Sciences, Wuhan Institute of Physics and Mathematics, State Key Laboratory of Catalysis, Innovation Academy for Precision Measurement Science and Technology, CAS
Language: English
Subfield: Inorganic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $5,380
OpenAlex ID: W3007517618