(521cg) Reaction Mechanism and Kinetics of Methanol Carbonylation on Atomically Dispersed ReOx/SiO2 from First Principles
AIChE Annual Meeting
2023
2023 AIChE Annual Meeting
Catalysis and Reaction Engineering Division
Poster Session: Catalysis and Reaction Engineering (CRE) Division
Wednesday, November 8, 2023 - 3:30pm to 5:00pm
In this work, we employ density functional theory, electronic structure analysis, and mean-field microkinetic modeling to explore the energy landscape of the system, reveal kinetically relevant steps and intermediates, and understand the origin of the superior performance of the ReOx/SBA-15 catalyst. We identify the redox reaction mechanism that is consistent with reported experimental reaction orders, apparent activation energy, reaction rate, and IR/XANES/EXAFS spectroscopic data. The importance of oxidation states and coordination numbers of a Re metal center is investigated and found to play a critical role in the reactivity of the proposed catalyst.
References
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