The constant increase of CO2 in the atmosphere requires immediate actions to limit it. Chemical activation and conversion of CO2 into clean fuels or commodities like CO, formate, or methanol is a promising strategy in ongoing efforts to achieve a sustainable global energy technology. The development of hybrid photoelectrodes comprised of molecular catalysts integrated with semiconducting light absorbers is desirable for coupling single photon absorptions to multi-electron/multi-proton liquid fuel production. Product selectivity during CO2 reduction can be controlled and directed by tuning the catalyst-semiconductor microenvironment on a molecular scale, tailoring proton activity, electric fields, dipoles and lipophilicity. Inter- and intramolecular strategies can be adopted: co-catalysts might be anchored on electrodes surfaces or embedded in the molecular structure of the catalyst itself. Both strategies have been adopted in this work, which investigates the role of cations for CO2 reduction using Re-bipyridine molecular catalysts. Tuning the second coordination sphere affects important parameters such as selectivity, overpotential, kinetics, catalytic mechanism, durability, turnover number (TON) and turnover frequency (TOF).

Tuning the catalyst microenvironment for CO2 electroreduction

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