There is a need to develop efficient chemical processes that can renewably generate ‘carbon-neutral’ chemicals and fuels, and our group has interest in elucidating fundamental mechanisms for efficiently reducing CO2. Growing numbers of electrochemical CO2 reduction studies have suggested that nitrogen-containing heterocycles such as imidazolium and pyridinium (both of which happen to be common cation species in ionic liquids) may be acting as co-catalysts that facilitate CO2 reduction into fuels and precursors for industrial chemicals. Numerous aspects of the proposed mechanisms for these processes remain unclear, but interestingly, first-principles quantum chemistry has highlighted that aromatic N-heterocycles maybe be an effective way to access energetically efficient and biomimetic proton/hydride transfer mechanisms. We present an overview of our group’s recent computational investigations that report Pourbaix diagrams derived from quantum chemistry modeling. These diagrams concisely present electrochemical environments that would facilitate conventional and biomimetic CO2 reduction mechanisms.

Pourbaix diagrams to guide searches for CO2 reduction catalysts

254th National Meeting (2017)

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