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Solar-driven liquid multi-carbon fuel production using a standalone perovskite–BiVO4 artificial leaf

Nature Energy volume 8, pages 629–638 (2023)Cite this article

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Abstract

The synthesis of high-energy-density liquid fuels from CO2 and H2O powered by sunlight has the potential to create a circular economy. Despite the progress in producing simple gaseous products, the construction of unassisted photoelectrochemical devices for liquid multi-carbon production remains a major challenge. Here we assembled artificial leaf devices by integrating an oxide-derived Cu94Pd6 electrocatalyst with perovskite–BiVO4 tandem light absorbers that couple CO2 reduction with water oxidation. The wired Cu94Pd6|perovskite–BiVO4 tandem device provides a Faradaic efficiency of ~7.5% for multi-carbon alcohols (~1:1 ethanol and n-propanol), whereas the wireless standalone device produces ~1 µmol cm−2 alcohols after 20 h unassisted operation under air mass 1.5 G irradiation with a rate of ~40 µmol h−1 gCu94Pd6−1. This study demonstrates the direct production of multi-carbon liquid fuels from CO2 over an artificial leaf and, therefore, brings us a step closer to using sunlight to generate value-added complex products.

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Fig. 1: Artificial leaf overview and physical characterization of the bimetallic catalyst.
Fig. 2: Electrochemical analysis of activated CuxPdy catalysts.
Fig. 3: Mechanistic analysis of multi-carbon production over activated Cu94Pd6 catalyst at low overpotentials.
Fig. 4: Unassisted multi-carbon alcohol production using wired tandem BiVO4–perovskite|Cu94Pd6 devices and wireless standalone artificial leaves.

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Data availability

The raw data supporting the findings of this study are available from the University of Cambridge data repository: https://doi.org/10.17863/CAM.95679.

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Acknowledgements

This work was supported by the European Commission with a Horizon 2020 Marie Skłodowska-Curie Individual European Fellowship (SolarFUEL, GAN 839763, M.R.), the Cambridge Trust (Vice-Chancellor’s Award to V.A., Cambridge Thai Foundation Award to C.P., HRH Prince of Wales Commonwealth Scholarship to S.B.), the Winton Programme for the physics of sustainability and St John’s College (Title A research fellowship to V.A.), the EPSRC (EP/L015978/1, EP/L027151/1, D.W., J.J.B., E.R.), the Swiss National Science Foundation (Early Postdoctoral Mobility fellowship P2EZP2-191791, E.L.) and the Austrian Science Fund (FWF, Schrödinger Fellowship J-4381, C.M.P). Access to the Cambridge XPS system, part of the Sir Henry Royce Institute-Cambridge equipment (EPSRC grant EP/P024947/1) and funding for TEM (EPSRC Underpinning Multi-User Equipment Call, EP/P030467/1) are gratefully acknowledged. We thank C. M. Fernández-Posada for assistance with the XPS and S. Kar and Y. Liu (University of Cambridge) for their valuable feedback on the paper.

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Authors and Affiliations

  1. Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK

    Motiar Rahaman, Virgil Andrei, Erwin Lam, Chanon Pornrungroj, Subhajit Bhattacharjee, Christian M. Pichler, Heather F. Greer & Erwin Reisner

  2. NanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of Cambridge, Cambridge, UK

    Demelza Wright & Jeremy J. Baumberg

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Contributions

M.R. and E.R. designed the project. M.R. developed the bimetallic catalyst, assembled the artificial leaf devices and performed all the (photo)electrochemical experiments. V.A. prepared and characterized the perovskite and BiVO4 light absorbers and made the supplementary video. D.W. performed the operando Raman experiments. E.L. carried out the DFT calculations. C.P. assisted with oxygen analysis and schematic diagrams. S.B. and C.M.P. assisted with the catalyst characterization and analytics. H.F.G. helped with electron microscopy analyses. J.J.B provided insights in Raman measurements. M.R. and E.R. collectively wrote the paper with input from all co-authors. E.R. supervised the work.

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Correspondence to Erwin Reisner.

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Nature Energy thanks Kazuhiro Takanabe and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–31, Tables 1–5 and References.

Supplementary Video 1

Evolution of gaseous products from photoanode and photocathode sides of a standalone artificial leaf under solar irradiation.

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Rahaman, M., Andrei, V., Wright, D. et al. Solar-driven liquid multi-carbon fuel production using a standalone perovskite–BiVO4 artificial leaf. Nat Energy 8, 629–638 (2023). https://doi.org/10.1038/s41560-023-01262-3

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