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Artificial photosynthesis: Lights off, gas on!

Nature Reviews Materials volume 2, Article number: 16102 (2017) Cite this article

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In natural photosynthesis, photoexcitation and effective charge separation facilitate spatially compartmentalized redox reactions in the electron-transport chain, generating NADPH and ATP. These molecules then drive a light-independent cycle to convert carbon dioxide to carbohydrates, oxygen and, in some species, hydrogen. Attempts to mimic these processes typically rely on complex electron relays to prevent electron–hole recombination and involve challenging synthesis methods. Consequently, the ‘artificial leaf’ is yet to find its way to market.

As the researchers report in Angewandte Chemie International Edition, these problems are overcome using cyanamide-functionalized heptazine-based carbon nitride. In previous work, they found that adding a cyanamide functionality to the heptazine units greatly improved the quantum efficiency for photocatalytic hydrogen evolution. Their latest study was conceived to further understand these observations. “Initially, our goal was to study the formation and role of ‘functional defects’, which may act as catalytically active sites in carbon nitride photocatalysts,” explains Lotsch. However, when they irradiated their polymer, they observed entirely unexpected behaviour: in the presence of a suitable electron donor, it underwent a colour change from yellow to a long-lived blue state, indicating the formation of a trapped radical species. “We had not foreseen that our synthetic approach would lead to carbon nitrides that can store a large number of reducing equivalents for long periods of time,” says Lotsch.

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References

  1. Lau, V. W.-h. et al. Dark photocatalysis: storage of solar energy in carbon nitride for time-delayed hydrogen generation. Angew. Chem. Int. Ed. http://dx.doi.org/10.1002/anie.201608553 (2016)

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  1. Adam Brotchie
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Brotchie, A. Artificial photosynthesis: Lights off, gas on!. Nat Rev Mater 2, 16102 (2017). https://doi.org/10.1038/natrevmats.2016.102

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  • DOI: https://doi.org/10.1038/natrevmats.2016.102

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