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Tailored self-assembled photocatalytic nanofibres for visible-light-driven hydrogen production

Abstract

The creation of efficient artificial systems that mimic natural photosynthesis represents a key current challenge. Here, we describe a high-performance recyclable photocatalytic core–shell nanofibre system that integrates a cobalt catalyst and a photosensitizer in close proximity for hydrogen production from water using visible light. The composition, microstructure and dimensions—and thereby the catalytic activity—of the nanofibres were controlled through living crystallization-driven self-assembly. In this seeded growth strategy, block copolymers with crystallizable core-forming blocks and functional coronal segments were coassembled into low-dispersity, one-dimensional architectures. Under optimized conditions, the nanofibres promote the photocatalytic production of hydrogen from water with an overall quantum yield for solar energy conversion to hydrogen gas of ~4.0% (with a turnover number of >7,000 over 5 h, a frequency of >1,400 h−1 and a H2 production rate of >0.327 μmol h−1 with 1.34 μg of catalytic polymer (that is, >244,300 μmol h−1 g−1 of catalytic polymer)).

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Fig. 1: Preparation and structures of self-assembled photocatalytic nanofibres.
Fig. 2: Characterization of self-assembled photocatalytic nanofibres.
Fig. 3: Photocatalytic HER performance of blend nanofibres.
Fig. 4: Steady-state absorption spectra and FLIM data for photocatalytic blend nanofibres.

Data availability

All of the data that support the findings of this study are available within the article and its Supplementary Information.

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Acknowledgements

Funding for this study was provided by a Marie Curie Fellowship (to J.T.), a European Research Council Advanced Grant (to I.M.) and a Canada 150 Research Chair and NSERC Discovery Grant (to I.M.). We thank the Wolfson Bioimaging Facility at the University of Bristol and additional funding from a BBSRC ALERT 13 capital grant (BB/L014181/1) and BrisSynBio, a BBSRC/EPSRC-funded Synthetic Biology Research Centre (grant L01386X). J.T. thanks J. D. Garcia-Hernandez and J. Dong for assistance with the LSCM experiments. We thank E. LaPierre for helpful discussions and J. Spence for assistance with the inductively coupled plasma mass spectrometry experiments.

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Contributions

J.T. and I.M. conceived the project. J.T., Y.Z., S.P. and Y.H. synthesized the materials. J.T. performed the experiments with assistance from the other authors. L.D., R.Y. and D.L.P. performed the fsTA studies. J.-C.E. performed the TEM and EDX imaging. R.L.H. performed the AFM analysis. D.A. performed the STED and FLIM imaging. J.T., I.M., X.-H.J. and Y.Z. contributed to data discussions. J.T. and I.M. analysed the data and wrote the manuscript with input from the other authors.

Corresponding author

Correspondence to Ian Manners.

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Supplementary information

Supplementary Information

Methods, polymer synthesis and characterization, block copolymer self-assembly, Supplementary Figs. 1–35, Supplementary Tables 1–4 and References.

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Tian, J., Zhang, Y., Du, L. et al. Tailored self-assembled photocatalytic nanofibres for visible-light-driven hydrogen production. Nat. Chem. 12, 1150–1156 (2020). https://doi.org/10.1038/s41557-020-00580-3

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