Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate. Issue 51 (2nd November 2016)

• Record Type: Journal Article
• Authors: Chowdhury, Abhishek Dutta; Houben, Klaartje; Whiting, Gareth T.; Mokhtar, Mohamed; Asiri, Abdullah M.; Al‐Thabaiti, Shaeel A.; Basahel, Suliman N.; Baldus, Marc; Weckhuysen, Bert M.
• Is Part Of: Angewandte Chemie international edition. Volume 55:Issue 51(2016)
• Page Start: 15840
• Page End: 15845
• Publication Date: 2016-11-02
• Subjects: methanol-to-olefin reaction -- operando spectroscopy -- reaction mechanisms -- solid-state NMR spectroscopy -- zeolites; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201608643
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: 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. Abstract : Direct formation of a C–C bond : By using a combination of UV/Vis spectroscopy, mass spectrometry, and advanced NMR spectroscopy, evidence was found for the formation of methyl acetate, dimethoxymethane and surface acetate species during the methanol‐to‐olefin (MTO) reaction over the zeolite catalyst H‐SAPO‐34. New insights in the formation of the first carbon–carbon bond during the MTO process are provided.