Covalent organic frameworks with high quantum efficiency in sacrificial photocatalytic hydrogen evolution

Chunzhi Li, Jiali Liu, He Li (), Kaifeng Wu, Junhui Wang () and Qihua Yang ()
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Chunzhi Li: Chinese Academy of Sciences
Jiali Liu: Chinese Academy of Sciences
He Li: Chinese Academy of Sciences
Kaifeng Wu: Chinese Academy of Sciences
Junhui Wang: Chinese Academy of Sciences
Qihua Yang: Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Organic semiconductors offer a tunable platform for photocatalysis, yet the more difficult exciton dissociation, compared to that in inorganic semiconductors, lowers their photocatalytic activities. In this work, we report that the charge carrier lifetime is dramatically prolonged by incorporating a suitable donor-acceptor (β-ketene-cyano) pair into a covalent organic framework nanosheet. These nanosheets show an apparent quantum efficiency up to 82.6% at 450 nm using platinum as co-catalyst for photocatalytic H2 evolution. Charge carrier kinetic analysis and femtosecond transient absorption spectroscopy characterizations verify that these modified covalent organic framework nanosheets have intrinsically lower exciton binding energies and longer-lived charge carriers than the corresponding nanosheets without the donor-acceptor unit. This work provides a model for gaining insight into the nature of short-lived active species in polymeric organic photocatalysts.

Date: 2022
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DOI: 10.1038/s41467-022-30035-x

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