Journal
ACS CATALYSIS
Volume 8, Issue 8, Pages 7356-7361Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02385
Keywords
methanol to olefins; induction period; carbon-carbon bond; direct mechanism; autocatalysis
Categories
Funding
- National Natural Science Foundation of China [91745109, 21473182, 91545104]
- Key Research Program of Frontier Sciences, CAS [QYZDY-SSW-JSC024]
- Youth Innovation Promotion Association of the Chinese Academy of Sciences [2014165]
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Methanol conversion during the induction period of methanol-to-olefin (MTO) process has been investigated by solid-state nuclear magnetic resonance (ssNMR), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), gas chromatography mass spectroscopy (GC-MS), and time-of-flight mass spectroscopy (TOF-MS), over HSAPO-34 molecular sieve. The two-dimensional (2D) C-13-C-13 MAS NMR spectra revealed the correlation of surface methoxy species (SMS) and dimethyl ether (DME)/methanol was enhanced with the temperature increase, supporting that the carbon carbon (C-C) bond can be possibly formed through the direct coupling of SMS and the surface-adsorbed Cl reactant. The evolution of surface species was monitored continuously by the aid of in situ ssNMR and in situ DRIFTS. With the consumption of SMS, alkenyl or/and phenyl carbocations were formed and accumulated as the successive intermediates for methanol conversion. Based on these direct observations, we propose that the first C-C bond is derived from SMS-mediated DME/methanol activation while alkenyl/phenyl carbocations can take over SMS and convert methanol efficiently in the autocatalysis stage of the MTO process.
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