Chemistry of CO2 to Bridge a Prebiotic Chemistry and Organic Synthesis

Carbon dioxide (CO2), traditionally regarded as an inert molecule, lies at the heart of the carbon cycle on and beneath the Earth's surface. Variations in atmospheric CO2 concentration have driven large fluctuations in global climate throughout Earth's history, while anthropogenic CO2 emissions are now recognized as one of the greatest challenges of our time. On the prebiotic Earth, atmospheric CO2 was far more abundant than it is today. Any reconstruction of the chemistry of that era is necessarily speculative, but the speculation is productive, because it directs attention to reaction scenarios that are unconventional by modern standards yet accessible under CO2-rich conditions. In this Account, we describe our efforts to bridge the chemistry of prebiotic CO2 with its utilization in modern organic synthesis. Fundamental studies inspired by prebiotic chemistry have led us to develop new synthetic methodologies, catalytic processes, and practical applications in which CO2 plays roles beyond that of a simple C1 feedstock. Through selected examples from our research, we illustrate how investigating the possible roles of CO2 in the origin of life can inspire new concepts and strategies for contemporary synthetic chemistry.