Artificial photosynthesis of alcohols from CO2 is still unsatisfactory owing to the rapid charge relaxation compared to the sluggish photoreactions and the oxidation of alcohol products. Here, we demonstrate that CO2 is reduced to methanol with 100 % selectivity using water as the only electron donor on a carbon nitride-like polymer (FAT) decorated with carbon dots. The quantum efficiency of 5.9 % (λ=420 nm) is 300 % higher than the previously reported carbon nitride junction. Using transient absorption spectroscopy, we observed that holes in FAT could be extracted by the carbon dots with nearly 75 % efficiency before they become unreactive by trapping. Extraction of holes resulted in a greater density of photoelectrons, indicative of reduced recombination of shorter-lived reactive electrons. This work offers a strategy to promote photocatalysis by increasing the amount of reactive photogenerated charges via structure engineering and extraction before energy losses by deep trapping.
Keywords: carbon dioxide fixation; carbon dots; charge trapping; photocatalysis; time-resolved spectroscopy.
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.