Abstract
Perovskite-based solar water splitting systems are promising candidates for addressing environmental challenges, exceeding the commercialization efficiency of solar-to-hydrogen (STH) at >10%. However, the operational stability remains suboptimal due to insufficient in situ/operando insights into charge carrier dynamics. Here, we investigate the role of charge accumulation on operational stability through operando catalytic modulation via near-infrared (NIR) toggling on a photothermal catalyst. Electrochemical analyses under operando NIR toggling demonstrate enhanced hydrogen evolution reaction kinetics and reduced charge recombination. In situ analyses confirm that reduced charge accumulation suppresses ion migration in the perovskite layer, thereby enhancing operational stability. The NIR-irradiated cathode delivers a photocurrent density of 25.48 mA cm–2, maintaining 90% of its initial photocurrent density at 0 VRHE for 310 h. A parallelly-illuminated coplanar system with NIR-irradiated perovskite-based water splitting cathode operates without bias, achieving a STH efficiency of 15.18%, retaining 70% of their initial performance for 115 h.
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Acknowledgements
This research was supported by National R&D Program through the National Research Foundation (NRF) of Korea (No. 2021R1A3B1068920 and 2021M3H4A1A03049662) funded by the Ministry of Science and ICT. This research was also supported by the Yonsei Signature Research Cluster Program of 2021 (2021-22-0002) and the Yonsei Fellowship, funded by Lee Youn Jae.
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C.-S.J. and J.M. conceived the idea and designed the cathode. C.-S.J., W.J., and J.Y. fabricated the perovskite-based electrodes and wrote the initial draft. W.J. and J.Y. conducted in-situ Raman spectroscopy and DLCP measurements, while J.Y. and C.-S.J. performed IMVS/IMPS tests and collected ex-situ data. C.-S.J. and W.J. analyzed the operando electrochemical data, and B.K. and C.-S.J. carried out high-speed profiling of bubble dynamics. D.K. and B.K. developed FEM modeling of Marangoni convection, with Hyungsoo L. and J.H.K. preparing the experimental setup. C.-S.J., W.J., J.W., B.K., D.K., Hyungsoo L., J.H.K., Hyungsuk L., and J.M. contributed to the discussion and revision of the manuscript. J.M. supervised the overall project.
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Jeong, CS., Jeong, W., Yun, J. et al. Operando insights into stability of perovskite-based solar water splitting devices. Nat Commun (2026). https://doi.org/10.1038/s41467-026-68357-9
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DOI: https://doi.org/10.1038/s41467-026-68357-9
