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Title: Monitoring the methanol conversion process in H-ZSM-5 using synchrotron X-ray powder diffraction-mass spectrometry

Journal Article · · Journal of Catalysis
 [1];  [1];  [2];  [2];  [3];  [1]
  1. Univ. of Oxford (United Kingdom)
  2. Harwell Science and Innovation Campus, Didcot (United Kingdom). Diamond Light Source, Ltd.
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
+ Show Author Affiliations

Using synchrotron X-ray powder diffraction-mass spectrometry in combination with theoretical calculations, we probed the structural changes of adsorbed methanol species in H-ZSM-5 for the first time during catalytic conversion of methanol. Preliminary experimental and computational findings suggested that associative mechanism was the dominant reaction pathway in the early stage of the reaction at 200 °C. Also, we observed a minor contribution from dissociative mechanism of the adsorbed methoxy intermediate species, CH3-Oz (where Oz is a framework oxygen atom), at Brønsted acid sites. In conclusion, it led to methoxy accumulation during the late stage of the reaction, which was postulated to be the initial step that produced ‘hydrocarbon pool’ and ‘coke’ through the formation of C$$-$$C bonds.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1543555
Alternate ID(s):
OSTI ID: 1495272; OSTI ID: 1582579
Journal Information:
Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 365; ISSN 0021-9517
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Chemistry
Engineering
Synchrotron X-ray powder diffraction-mass spectrometry
Methanol conversion
Density functional theory
H-ZSM-5 zeolites
Carbon deposition