Abstract
Dimethyl ether (DME) carbonylation is an important intermediate step in the synthesis of methyl acetate (MA) and ethanol. H-form mordenite (MOR) can efficiently catalyze the reaction, in which Brønsted acid sites (BASs) associated with framework Al function as active sites. But the role of other Al species such as exteraframework Al (EFAl) and framework-associated Al still remains unknown. In this study, we have proposed two convenient approaches for controlling the two Al species and investigating their influence on the DME carbonylation reaction. NH3-TPD and Py-IR analyses revealed that the number of BASs increased after the removal of EFAl and the inhibition the formation of framework-associated Al. The reactivity results showed that the elimination of EFAl promoted the DME conversion from 28% to 46%. Additionally, through the implementation of in-situ calcination to impede the presence of framework-associated Al, the DME conversion increased from 28% to 50%. With the understanding that both EFAl and framework-associated Al have a detrimental effect on the reaction, the highest conversion is achieved with these two treatments, leading to 73% DME conversion with 99% selectivity to MA. Our findings provide a systematical strategy to effectively regulate the presence of Al species in zeolite, offering insights of rational design to optimize zeolite catalysts for important industrialized process.
Accepted Version (Free)
Published Version
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.