Metal-free reduction of CO2 to formate using a photochemical organohydride-catalyst recycling strategy

Abstract

Increasing levels of CO₂ in the atmosphere is a problem that must be urgently resolved if the rise in current global temperatures is to be slowed. Chemically reducing CO₂ into compounds that are useful as energy sources and carbon-based materials could be helpful in this regard. However, for the CO₂ reduction reaction (CO₂RR) to be operational on a global scale, the catalyst system must: use only renewable energy, be built from abundantly available elements and not require high-energy reactants. Although light is an attractive renewable energy source, most existing CO₂RR methods use electricity and many of the catalysts used are based on rare heavy metals. Here we present a transition-metal-free catalyst system that uses an organohydride catalyst based on benzimidazoline for the CO₂RR that can be regenerated using a carbazole photosensitizer and visible light. The system is capable of producing formate with a turnover number exceeding 8,000 and generates no other reduced products (such as H₂ and CO).