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Unraveling the Homologation Reaction Sequence of the Zeolite-Catalyzed Ethanol-to-Hydrocarbons Process.


ABSTRACT: Although industrialized, the mechanism for catalytic upgrading of bioethanol over solid-acid catalysts (that is, the ethanol-to-hydrocarbons (ETH) reaction) has not yet been fully resolved. Moreover, mechanistic understanding of the ETH reaction relies heavily on its well-known "sister-reaction" the methanol-to-hydrocarbons (MTH) process. However, the MTH process possesses a C1 -entity reactant and cannot, therefore, shed any light on the homologation reaction sequence. The reaction and deactivation mechanism of the zeolite H-ZSM-5-catalyzed ETH process was elucidated using a combination of complementary solid-state NMR and operando UV/Vis diffuse reflectance spectroscopy, coupled with on-line mass spectrometry. This approach establishes the existence of a homologation reaction sequence through analysis of the pattern of the identified reactive and deactivated species. Furthermore, and in contrast to the MTH process, the deficiency of any olefinic-hydrocarbon pool species (that is, the olefin cycle) during the ETH process is also noted.

SUBMITTER: Chowdhury AD 

PROVIDER: S-EPMC6519145 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Unraveling the Homologation Reaction Sequence of the Zeolite-Catalyzed Ethanol-to-Hydrocarbons Process.

Chowdhury Abhishek Dutta AD   Lucini Paioni Alessandra A   Whiting Gareth T GT   Fu Donglong D   Baldus Marc M   Weckhuysen Bert M BM  

Angewandte Chemie (International ed. in English) 20190214 12


Although industrialized, the mechanism for catalytic upgrading of bioethanol over solid-acid catalysts (that is, the ethanol-to-hydrocarbons (ETH) reaction) has not yet been fully resolved. Moreover, mechanistic understanding of the ETH reaction relies heavily on its well-known "sister-reaction" the methanol-to-hydrocarbons (MTH) process. However, the MTH process possesses a C<sub>1</sub> -entity reactant and cannot, therefore, shed any light on the homologation reaction sequence. The reaction a  ...[more]

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