NMR Computational Studies of Solid Acidity/Fundamental Studies of Catalysis by Solid Acids
This project focused on catalysis by zeolites and the synergy of spectroscopic characterization and theoretical modeling. In collaboration with the Waroquier group in Belgium we used state-of-the-art quantum chemical simulations on a supramolecular model of both the HZSM-5 zeolite and the co-catalytic hydrocarbon pool species and calculated a full catalytic cycle (including all rate constants) for methanol-to-olefin (MTO) catalysis involving a hydrocarbon pool species. This work not only represents the most robust computational analysis of a successful MTO route to date, but it also succeeds in tying together the many experimental clues. That work was featured on the cover of Angewandte Chemie. More recently we elucidated several unsuspected roles for formaldehyde in methanol to olefin catalysis. Formaldehyde proves to be a key species responsible for both the growth of the catalytically active hydrocarbon pool and its inevitable aging into deactivated polycyclic aromatic species. The apparent inevitability of formaldehyde formation at high temperatures, in particular in contact with active metal or metal oxide surfaces, may put some fundamental limitations on the economic potential of conversion of methanol to olefins.
- Research Organization:
- University of Southern California, Los Angeles, CA
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- FG02-99ER14956
- OSTI ID:
- 1049372
- Report Number(s):
- DOE/ER/14956-1
- Country of Publication:
- United States
- Language:
- English
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