Abstract
The activity and selectivity of simple photocatalysts for CO2 reduction remain limited by the insufficient photophysics of the catalysts, as well as the low solubility and slow mass transport of gas molecules in/through aqueous solution. In this study, these limitations are overcome by constructing a triphasic photocatalytic system, in which polymeric carbon nitride (CN) is immobilized onto a hydrophobic substrate, and the photocatalytic reduction reaction occurs at a gas–liquid–solid (CO2–water–catalyst) triple interface. CN anchored onto the surface of a hydrophobic substrate exhibits an approximately 7.2‐fold enhancement in total CO2 conversion, with a rate of 415.50 μmol m−2 h−1 under simulated solar light irradiation. This value corresponds to an overall photosynthetic efficiency for full water–CO2 conversion of 0.33 %, which is very close to biological systems. A remarkable enhancement of direct C2 hydrocarbon production and a high CO2 conversion selectivity of 97.7 % are observed. Going from water oxidation to phosphate oxidation, the quantum yield is increased to 1.28 %.
Highlights
The activity and selectivity of simple photocatalysts for CO2 reduction remain limited by the insufficient photophysics of the catalysts, as well as the low solubility and slow mass transport of gas molecules in/through aqueous solution
Previous studies found that the availability of excess protons (H+) and low concentration of CO2 at the reaction interface lead to unsatisfactory activity and selectivity of the photocatalytic CO2 reduction system.[8]
After carbon nitride (CN) immobilization on one side of the substrate, the side with the CN layer becomes superhydrophilic or hydrophilic with contact angles (CAs) of approximately 08, 08 and 108
Summary
The activity and selectivity of simple photocatalysts for CO2 reduction remain limited by the insufficient photophysics of the catalysts, as well as the low solubility and slow mass transport of gas molecules in/through aqueous solution. The kinetics of catalysts and CO2 photoreduction efficiency.[3] the competitive reaction of photocatalytic hydrogen evolution diminishes the generation of hydrocarbons, resulting in low selectivity and activity of CO2 reduction of most current systems.
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