(172c) DFT Study on the Catalytic Activity of Oxo-Centered Trimetallic MOF Building Units for Ethane Oxidation to Ethanol
AIChE Annual Meeting
2018 AIChE Annual Meeting
Catalysis and Reaction Engineering Division
Rational Catalyst Design II
Monday, October 29, 2018 - 1:10pm to 1:30pm
To examine the catalytic activity of oxo-centered trimetallic MOF nodes, we used density functional theory (DFT) to model the three main steps involved in the conversion of ethane to ethanol using N2O as the oxidant: (1) N2O activation, (2) C-H activation, and (3) ethanol desorption. Our results show that the N2O activation step is the rate determining step for the reaction to proceed.
Analysis of the electron orbital occupation reveals that this energy barrier gets higher as the d-orbitals of the active metal become more populated. This indicates that the electrons in high-energy molecular orbitals are easier to oxidize and the oxygen atom in N2O binds more strongly. Thus, we find that the oxygen binding strength and energy of the highest occupied molecular orbital (HOMO) describe well the catalytic activity of these clusters and are plausible descriptors that we can use to screen for a larger sample of catalysts.