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All-perovskite-based unassisted photoelectrochemical water splitting system for efficient, stable and scalable solar hydrogen production

Nature Energy volume 9, pages 272–284 (2024)Cite this article

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Abstract

For practical photoelectrochemical water splitting to become a reality, highly efficient, stable and scalable photoelectrodes are essential. However, meeting these requirements simultaneously is a difficult task, as improvements in one area can often lead to deteriotation in others. Here, addressing this challenge, we report a formamidinium lead triiodide (FAPbI3) perovskite-based photoanode that is encapsulated by an Ni foil/NiFeOOH electrocatalyst, which demonstrates promising efficiency, stability and scalability. This metal-encapsulated FAPbI3 photoanode records a photocurrent density of 22.8 mA cm−2 at 1.23 VRHE (where VRHE is voltage with respect to the reversible hydrogen electrode) and shows excellent stability for 3 days under simulated 1-sun illumination. We also construct an all-perovskite-based unassisted photoelectrochemical water splitting system by connecting the photoanode with a same-size FAPbI3 solar cell in parallel, which records a solar-to-hydrogen efficiency of 9.8%. Finally, we demonstrate the scale-up of these Ni-encapsulated FAPbI3 photoanodes into mini-modules up to 123 cm2 in size, recording a solar-to-hydrogen efficiency of 8.5%.

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Fig. 1: NiFeOOH/Ni/FAPbI3 photoanode and all-PSK-based en-PEC mini-module.
Fig. 2: Structure and performance of the n–i–p-structured FAPbI3 PV cell.
Fig. 3: Device structure and PEC performance of the n–i–p-configured NiFeOOH/Ni/FAPbI3 photoanode.
Fig. 4: Charge transport, separation and transfer kinetics of OEC/Ni/FAPbI3 photoanodes using different OECs (NiFeOOH, NiOOH and FeOOH) and their effects on the activity and stability of the photoanodes.
Fig. 5: Scale-up demonstration of the NiFeOOH/Ni/FAPbI3 photoanode mini-module for an unassisted PEC water splitting system.

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Data availability

All data generated or analysed during this study are included in the published article. The experimental data for all the supplementary figures are provided as Supplementary Data. Source data are provided with this paper.

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Acknowledgements

This work was supported by the Climate Change Response Project (NRF-2019M1A2A2065612), the Brainlink Project (NRF-2022H1D3A3A01081140 and NRF-2021R1A4A3027878) (awarded to J.S.L.) and the Basic Science Research Program (NRF-2018R1A3B1052820) (awarded to S.I.S.) funded by the Ministry of Science and ICT of Korea via the National Research Foundation, and by research funds from Hanhwa Solutions Chemicals (1.220029.01), UNIST (1.190013.01) (awarded to J.S.L. and J.-W.J.) and the Carbon Neutrality Demonstration and Research Centre at UNIST (1.230053.01) (awarded to H.L.). This work was also supported by the Institute for Basic Science (IBS-R019-D1) and the Alchemist Project 1415184376 (20019321) (awarded to J.-W.J.). The authors are grateful to the instrumentation facility at the UNIST Central Research Facility.

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  1. These authors contributed equally: Dharmesh Hansora, Jin Wook Yoo, Rashmi Mehrotra.

Authors and Affiliations

  1. Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology, Ulsan, Republic of Korea

    Dharmesh Hansora, Jin Wook Yoo, Rashmi Mehrotra, Woo Jin Byun, Dongjun Lim, Young Kyeong Kim, Eunseo Noh, Hankwon Lim, Ji-Wook Jang, Sang Il Seok & Jae Sung Lee

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Contributions

D.H., J.W.Y., J.-W.J., S.I.S. and J.S.L. designed and directed the research. D.H. conceived the concept of stabilizing FAPbI3 PSK photoanodes using metal encapsulation. J.W.Y. and E.N. prepared the FAPbI3 PV cells and mini-modules and measured their performance. D.H. and R.M. stabilized and protected small and scaled-up FAPbI3 PEC cells and measured their performance with characterization. W.J.B. conducted GC analysis, while Y.K.K. synthesized and characterized the NiFeOOH electrocatalyst for the OER experiments. D.H., R.M. and W.J.B. designed and fabricated the PEC reactor using acrylic components at Makelab at UNIST. D.L. and H.L. performed the techno-economic analysis. D.H., J.W.Y., R.M., J.-W.J., S.I.S. and J.S.L. co-wrote the paper. All authors read and commented on the paper.

Corresponding authors

Correspondence to Hankwon Lim, Ji-Wook Jang, Sang Il Seok or Jae Sung Lee.

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Competing interests

D.H., R.M., W.J.B., J.-W.J. and J.S.L. prepared a Korean patent application (10-2023-0196699 dated 2023-12-29) concurrently with this paper. The other authors declare no competing interests.

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Nature Energy thanks Jing Gu, Gerko Oskam, Ludmilla Steier 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 Figs. 1–38, Tables 1–8, Notes 1–10 and references.

Supplementary Data 1

Techno-economic analyses (TEA) calculations.

Supplementary Data 2

Source data for supplementary figures.

Supplementary Video 1

Multi-cell PEC system (7.68 and 30.8 cm2).

Supplementary Video 2

Multi-reactor PEC system (123 cm2).

Source data

Source Data Fig. 2

Source data for Fig. 2.

Source Data Fig. 3

Source data for Fig. 3 and statistical source data for Fig. 3e.

Source Data Fig. 4

Source data for Fig. 4.

Source Data Fig. 5

Source data for Fig. 5 and statistical source data for Fig. 5c.

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Hansora, D., Yoo, J.W., Mehrotra, R. et al. All-perovskite-based unassisted photoelectrochemical water splitting system for efficient, stable and scalable solar hydrogen production. Nat Energy 9, 272–284 (2024). https://doi.org/10.1038/s41560-023-01438-x

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