Proton-Coupled Electronic Processes

Proton-coupled electron transfer (PCET) has become recognized as a fundamental reaction of fundamental importance in broad areas of chemistry and biology and of practical importance for e.g. organic (photo)redox catalysis and catalytic production of solar- and electro-fuels.My group recently discovered (Science 2022) a new elementary reaction that we denoted Proton-coupled energy transfer (PCEnT).

We suggested that PCEnT may be commonly occurring and have interesting applications, but our understanding of this reaction is preliminary and further studies are needed.Fundamental studies of molecular model systems were crucial to develop an understanding of electron transfer, and for related applications.

Studies of model systems for PCET and PCEnT are similarly important for these processes.

I will take advantage of my recent progress and new methods, to reach the following overall aims:To increase our understanding of the newly discovered PCEnT reaction and its potential, and explore and broaden the scope of PCEnT reactivity.To establish the predicted driving force dependence of PCET, and resolve experimental and conceptual disagreements on PCET for C-H and N-H activation by photoredox catalysis.To experimentally characterize and manipulate the manifold of vibronic transitions involved in PCET reactions and coupled vibrations, and their correlation to PCET reactivity.