(230a) Tuning Selective Interactions with Free-Atom-like States on Single Atom Alloys
AIChE Annual Meeting
Tuesday, November 15, 2022 - 8:00am to 8:20am
In the limit of very dilute alloyingâthe so-called âsingle-atom-alloyâ (SAA) regimeâcertain bimetallic systems exhibit weak mixing between constituent metal wavefunctions, resulting in sharp, single-atom-like electronic states localized on the dilute component of the alloy. This work shows that when these sharp states are appropriately positioned in energy relative to given molecular orbitals, selective hybridization is enhanced, in accordance with intuitive principles of molecular orbital theory. We demonstrate the phenomenon for activation pathways of crotonaldehyde, a model Î±, Î²-unsaturated aldehyde, which can be representative of moieties in biomass feedstocks or derived from aldol condensation of acetaldehyde, a green product of CO2RR or biomass derived ethanol oxidation. The mechanistic understanding gathered can be used to steer selectivity towards highly synthetically valuable unsaturated alcohols. The link between in-silico design and early experimental results will be discussed.