One of the greatest challenges in catalysis research is selectivity, i.e., production of a desired product over an undesired one. The oxidation of n-butane to 1-butanol is important in the fuel and pharmaceuticals industries, but selectivity is a challenge for at least three reasons: 1) CO2 and H2O are thermodynamically preferred over butanol, 2) 2-butanol is more thermodynamically favorable than 1-butanol, and 3) 1-butanal is more thermodynamically favorable than 1-butanol. Designing a catalyst and set of reaction conditions for production of 1-butanol thus requires a catalyst that kinetically inhibits oxidation of butane's secondary carbon and overoxidation of its primary carbon. Herein, we explore properties of bimetallic catalysts that achieve such kinetic control. Specifically, we use density functional theory (DFT) along with microkinetic modeling and computational catalyst screening to identify catalyst properties and reaction conditions that have the potential to promote high activity and selectivity to 1-butanol. We find that high activity and selectivity toward 1-butanol can be achieved at low partial pressures of O2 and when H2O is co-fed as an oxidant over catalysts that balance affinity for C*, OH*, and O*. Making these discoveries required significant attention to detail and letting results guide new hypotheses, things that emanate from the work of Prof. Nikolla.

Reaction pathways and microkinetic modeling of n-butane oxidation to 1-butanol on Cu, Cu3Pd, Pd, Ag3Pd, and PdZn (111) surfaces

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.