(509z) Combining Metal Sulfides and Organic Cocatalysts to Overcome the Challenges of Electrochemical CO2 Reduction
AIChE Annual Meeting
2021
2021 Annual Meeting
Catalysis and Reaction Engineering Division
Poster Session: Catalysis and Reaction Engineering (CRE) Division
Wednesday, November 10, 2021 - 3:30pm to 5:00pm
We have used DFT to calculate barriers on such a cocatalyst, 1,3-dimethylimidazolium (DMIM), and found that CO2 can be activated by this molecule through electron-coupled addition to the carbon in the 2-position of the aromatic ring. The activated complex then undergoes several proton-coupled electron transfer steps and decomposes to eliminate CO. However, the activation barriers for this pathway are also too high for it to proceed at reasonable temperatures when the cocatalyst is not electronically coupled to the electrode. We further hypothesize that the DMIM cocatalyst chemisorbs on the MoS2 surface so that hybridization between the cocatalyst and surface orbitals lowers the electron transfer barriers enough for the proposed pathway to occur.