Initial Carbon-Carbon Bond Formation during the Early Stages of the Methanol-to-Olefin Process Proven by Zeolite-Trapped Acetate and Methyl Acetate.
Methanol-to-olefin (MTO) catalysis is a very active field of research because there is a wide variety of sometimes conflicting mechanistic proposals. An example is the ongoing discussion on the initial C-C bond formation from methanol during the induction period of the MTO process. By employing a combination of solid-state NMR spectroscopy with UV/Vis diffuse reflectance spectroscopy and mass spectrometry on an active H-SAPO-34 catalyst, we provide spectroscopic evidence for the formation of surface acetate and methyl acetate, as well as dimethoxymethane during the MTO process. As a consequence, new insights in the formation of the first C-C bond are provided, suggesting a direct mechanism may be operative, at least in the early stages of the MTO reaction.
Inorganic Chemistry and Catalysis group Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
Abhishek Dutta
AD
Chowdhury
NMR Spectroscopy, Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH, Utrecht, The Netherlands.
Klaartje
K
Houben
Inorganic Chemistry and Catalysis group Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
Gareth T
GT
Whiting
Department of Chemistry, King Abdulaziz University, P.O. Box 80203, 21589, Jeddah, Saudi Arabia.
Mohamed
M
Mokhtar
Department of Chemistry, King Abdulaziz University, P.O. Box 80203, 21589, Jeddah, Saudi Arabia.
Abdullah M
AM
Asiri
Department of Chemistry, King Abdulaziz University, P.O. Box 80203, 21589, Jeddah, Saudi Arabia.
Shaeel A
SA
Al-Thabaiti
Department of Chemistry, King Abdulaziz University, P.O. Box 80203, 21589, Jeddah, Saudi Arabia.
Suliman N
SN
Basahel
NMR Spectroscopy, Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH, Utrecht, The Netherlands.
Marc
M
Baldus
Inorganic Chemistry and Catalysis group Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
Bert M
BM
Weckhuysen
methanol-to-olefin reaction; operando spectroscopy; reaction mechanisms; solid-state NMR spectroscopy; zeolites