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Floating perovskite-BiVO4 devices for scalable solar fuel production

Abstract

Photoelectrochemical (PEC) artificial leaves hold the potential to lower the costs of sustainable solar fuel production by integrating light harvesting and catalysis within one compact device. However, current deposition techniques limit their scalability1, whereas fragile and heavy bulk materials can affect their transport and deployment. Here we demonstrate the fabrication of lightweight artificial leaves by employing thin, flexible substrates and carbonaceous protection layers. Lead halide perovskite photocathodes deposited onto indium tin oxide-coated polyethylene terephthalate achieved an activity of 4,266 µmol H2 g−1 h−1 using a platinum catalyst, whereas photocathodes with a molecular Co catalyst for CO2 reduction attained a high CO:H2 selectivity of 7.2 under lower (0.1 sun) irradiation. The corresponding lightweight perovskite-BiVO4 PEC devices showed unassisted solar-to-fuel efficiencies of 0.58% (H2) and 0.053% (CO), respectively. Their potential for scalability is demonstrated by 100 cm2 stand-alone artificial leaves, which sustained a comparable performance and stability (of approximately 24 h) to their 1.7 cm2 counterparts. Bubbles formed under operation further enabled 30–100 mg cm−2 devices to float, while lightweight reactors facilitated gas collection during outdoor testing on a river. This leaf-like PEC device bridges the gulf in weight between traditional solar fuel approaches, showcasing activities per gram comparable to those of photocatalytic suspensions and plant leaves. The presented lightweight, floating systems may enable open-water applications, thus avoiding competition with land use.

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Fig. 1: The thin perovskite-BiVO4 artificial leaf and its components.
Fig. 2: (Photo)electrochemistry of the GE electrodes, thin perovskite and BiVO4 photoelectrodes.
Fig. 3: Performance of scalable lightweight photoelectrodes and PEC devices for solar fuel production.

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Data availability

The raw data that support the findings of this study are available from the University of Cambridge data repository41: https://doi.org/10.17863/CAM.82770.

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Acknowledgements

This work was supported by the OMV group (to V.A., C.P., A.W. and E.R.); the Cambridge Trust (Vice-Chancellor’s Award to V.A. and Cambridge Thai Foundation Award to C.P.); the Winton Programme for the Physics of Sustainability and Cambridge Philosophical Society (to V.A.); Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq grant no. 204123/2017-8 to G.M.U.); a Trinity-Henry Barlow Scholarship (to C.P.); an EU Marie Sklodowska-Curie individual Fellowship (no. GAN 793996 to Q.W.); Christian Doppler Research Association, the Austrian Federal Ministry for Digital and Economic Affairs, and the National Foundation for Research, Technology and Development (to D.S.A., H.K., A.W. and E.R.); EPSRC Department Training Partnership studentship (EP/N509620/1) and B. Welland (to R.A.J.); Thailand’s Institute for the Promotion of Teaching Science and Technology Scholarship (to C.U.); the Herchel Smith Research Fund (to S.D.P.); the EPSRC Cambridge NanoDTC (nos. EP/L015978/1 and EP/S022953/1 to T.L. and E.R.); the Royal Academy of Engineering via the Research Fellowships scheme (no. RF\201718\1701 to R.L.Z.H.); the Royal Academy of Engineering Chair in Emerging Technologies scheme (no. CIET1819_24 to J.L.M.-D.); European Research Council Grants ‘MatEnSAP’ (no. 682833 to Q.W., K.P.S. and E.R.) and ‘ACrossWire’(no. 716471 to H.J.J.). We thank M. Woolley (University of Cambridge, Technical Services) for aid in constructing the large-scale reactors. We also thank S. D. Stranks, M. Rahaman and T. Li (University of Cambridge) for useful feedback on the manuscript.

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Authors and Affiliations

Authors

Contributions

V.A., G.M.U., R.L.Z.H., R.H.F. and E.R. designed the project. V.A. and G.M.U. conducted (photo)electrochemical characterization. V.A., R.A.J. and R.L.Z.H. developed the perovskite solar cells. V.A., Q.W. and C.P. developed the BiVO4 photoanodes. V.A. developed the large-scale samples and PEC reactors. C.U. conducted parylene-C deposition. H.L., S.D.P. and D.S.W. synthesized the single-source precursors. D.S.A. conducted TGA characterization. D.S.A. and H.K. provided support on the photocatalytic part. V.A. performed O2 quantification with support from K.P.S. V.A. developed the GE encapsulation, T.L. aided with preliminary tests. A.W. provided GC assistance. V.A. drafted the manuscript. V.A., G.M.U., C.P., Q.W., D.S.A., H.K., K.P.S., R.A.J., C.U., H.L., T.L., A.W., S.D.P., D.S.W., H.J.J., R.L.Z.H., J.L.M.-D., R.H.F. and E.R. contributed to the discussion, revision and completion of the manuscript. E.R. supervised the work.

Corresponding author

Correspondence to Erwin Reisner.

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Nature thanks Reiner Sebastian Sprick, Ryu Abe and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Tables 1–6, Figs. 1–51, Discussions 1 and 2 and references. Items provide additional data, plots and photographs related to the work.

Supplementary Video 1

Light-driven fuel production using wired thin perovskite photocathodes and small-scale PEC devices. A 1.7 cm2 Ti|BiVO4|TiCo–fPVK|GE|CoMTPP@CNT PEC device achieved buoyancy three consecutive times. Experiments are further described in the video subtitles and Supplementary Figs. 41 and 42.

Supplementary Video 2

Scalable unassisted fuel production using stand-alone 100 cm2 lightweight PEC devices with Pt and CoMTPP@CNT catalysts. Experiments are described in the video subtitles and Supplementary Fig. 42.

Supplementary Video 3

Ignition tests for 2:1 H2:O2 gas mixtures in sealed reactors. Experiments are described in video subtitles and Supplementary Fig. 48.

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Andrei, V., Ucoski, G.M., Pornrungroj, C. et al. Floating perovskite-BiVO4 devices for scalable solar fuel production. Nature 608, 518–522 (2022). https://doi.org/10.1038/s41586-022-04978-6

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