Valorization of CO₂ and N₂O Gas Enabled by a Single Multi-Photoinduced Electron Transfer Catalyst

The valorization of greenhouse gases CO₂ and N₂O into value-added chemicals has recently become a critical area of research. While the utilization of CO₂ gives quick access to important carboxylic acid building blocks, N₂O is able to act as an oxygen-transfer reagent that allows the formation of carbon-oxygen and heteroatom-oxygen bonds. No metal-free catalytic system has yet been described that is able to react with both gases. Additionally, the metal-free catalytic activation of N₂O is unprecedented in the literature. Relying on our previously established multi-PET catalysis that makes use of a BOIMPY dye, we were able to identify a single catalytic platform that allows reactions of both gases under super-reducing photochemical conditions. In this work, we report reactions between either CO₂ or N₂O and (poly)arenes, aryl halides, olefins, sulfides, and phosphines and present a thorough mechanistic investigation to understand the pathways leading to the described products. We found that N₂O is indeed catalytically activated by a nonmetal catalyst for the first time employing our system. We mention that the enclosed methodology can be utilized to react with abundant CO₂ or N₂O; however, it will not mitigate climate change.