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Conformally coated scaffold design using water-tolerant Pr1.8Ba0.2NiO4.1 for protonic ceramic electrochemical cells with 5,000-h electrolysis stability

Nature Energy volume 10, pages 890–903 (2025)Cite this article

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Abstract

Protonic ceramic electrochemical cells (PCECs) have potential as long-duration energy storage systems. However, their operational stability is limited under industrially relevant conditions due to the intrinsic chemical instability of doped barium cerate-based electrolytes and oxygen electrodes against H2O, as well as the poor electrode–electrolyte interfacial contact. Here we present a conformally coated scaffold (CCS) design to comprehensively address these issues. A porous proton-conducting scaffold is constructed and conformally coated with Pr1.8Ba0.2NiO4.1 electrocatalyst, which has high chemical stability against H2O, triple conductivity and hydration capability, and protects vulnerable electrolytes from H2O. The CCS structure consolidates the electrode–electrolyte interfacial bonding to enable fast proton transfer in the percolated network. This design enables PCECs to reach electrolysis stability for 5,000 h at −1.5 A cm−2 and 600 °C in 40% H2O. This work provides a general strategy to stabilize PCECs and offers guidance for designing resilient and stable solid-state energy storage systems.

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Fig. 1: Illustration of fabrication methods for PCECs and their degradation mechanism.
Fig. 2: Materials characterization.
Fig. 3: Electrochemical performances of the PCECs with CCS electrodes.
Fig. 4: Multiscale multiphysics modelling and computations for the CCS-based air electrode in EC mode.
Fig. 5: Electrochemical performance of the developed PBNO-BZCYYb1711 CCS-based UR-PCEC.

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Data availability

All of the data supporting the findings of this study are available within this Article and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

X. Liu acknowledges funding from the US Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) under contract no. DE-E0008378. We thank the technology managers N. Stetson, D. Peterson and W. Gibbons for technical guidance and financial support. J.L. and K.H. jointly acknowledge partial support by the National Science Foundation Materials Research Science and Engineering Center programme through the University of California Irvine Center for Complex and Active Materials (DMR-2011967). K.H. and H.Z. acknowledge support by the National Science Foundation through the CAREER programme (DMR-2239598) and the use of facilities and instrumentation at the University of California Irvine Materials Research Institute (IMRI), supported in part by the National Science Foundation Materials Research Science and Engineering Center programme through the UC Irvine Center for Complex and Active Materials (DMR-2011967). G.L. and Xiaolin Li acknowledge the US Department of Energy, Office of Electricity (Pacific Northwest National Laboratory project number 70247) for supporting 3D XRM instrumentation and characterization. M.R.R. and F.X. acknowledge the Australian Research Council for funding the in situ XRD instrument through project LE170100199. M.K. acknowledges Murdoch University for providing a Murdoch International Postgraduate Scholarship (MIPS). The use of the WVU Shared Research Facilities is acknowledged. H.T. thanks C. Li at Xi’an Jiaotong University for technical suggestions on cell fabrication and testing. We thank L. Hu at the University of Maryland, College Park and Yale University for technical discussions.

Author information

Authors and Affiliations

  1. Department of Mechanical, Materials and Aerospace Engineering, Benjamin M. Statler College of Engineering and Mineral Resources, West Virginia University, Morgantown, WV, USA

    Hanchen Tian, Wei Li, Qingyuan Li, Liang Ma, Xiujuan Chen, Yi Wang, Cijie Liu & Xingbo Liu

  2. State Key Laboratory for Mechanical Behavior of Materials, School of Materials Science and Engineering, Xi’an Jiaotong University, Xi’an, China

    Hanchen Tian & Zhuozhao Shao

  3. National Energy Technology Laboratory, Pittsburgh, PA, USA

    Yueh-Lin Lee & Wissam A. Saidi

  4. NETL Support Contractor, Pittsburgh, PA, USA

    Yueh-Lin Lee

  5. Department of Materials Science and Engineering, University of California, Irvine, CA, USA

    Hongkui Zheng & Kai He

  6. School of Materials Science and Engineering, Hebei University of Engineering, Handan, China

    Liang Ma

  7. Department of Chemical and Biomedical Engineering, Benjamin M. Statler College of Engineering and Mineral Resources, West Virginia University, Morgantown, WV, USA

    Debangsu Bhattacharyya, Wenyuan Li & Xuemei Li

  8. Program in Materials Science and Engineering, University of California San Diego, La Jolla, CA, USA

    Dawei Zhang & Jian Luo

  9. Battery Materials and Systems Group, Pacific Northwest National Laboratory, Richland, WA, USA

    Guosheng Li & Xiaolin Li

  10. Bavarian Center for Battery Technology (BayBatt), Department of Chemistry, University of Bayreuth, Bayreuth, Germany

    Li Li & Qingsong Wang

  11. School of Mathematics, Statistics, Chemistry and Physics, Murdoch University, Perth, Western Australia, Australia

    Fang Xia & Muhammet Kartal

  12. John de Laeter Centre, Curtin University, Perth, Western Australia, Australia

    Matthew R. Rowles

  13. Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California San Diego, La Jolla, CA, USA

    Jian Luo

Authors
  1. Hanchen Tian
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  2. Wei Li
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Contributions

X. Liu led the project, directed the formulation of overarching project goals, acquired the financial support and supervised the project. H.T., Wenyuan Li and X. Liu conceived the original concept of conformally coated scaffold design. Wei Li conceived the concept of unitized regenerative protonic ceramic electrochemical cell applications for long-duration energy storage cycling and seawater electrolysis. H.T. and Wei Li directed the evolution of the research planning and execution designed the screening criteria for materials, device fabrication, experiments and methodology, fabricated the cells, conducted most of the electrochemical, chemical, material and post-mortem characterizations, performed the CFD modelling, analysed the data and prepared most of the figures. Y.-L.L. conducted the DFT and AIMD calculations and prepared related figures. H.Z. and K.H. performed most of the TEM characterizations and analysis. Q.L. contributed to the electrochemical characterization of symmetric cells and part of the materials characterization. L.M. performed part of the electrochemical characterizations and assisted in the fabrication of the button and large cells and process development and optimization. D.B. conducted the technoeconomic analysis and wrote the related discussion. X.C. performed part of the materials characterization. D.Z. and J.L. contributed to part of the TEM characterizations. G.L. and Xiaolin Li contributed to the XRM characterizations. Y.W. assisted in part of the electrochemical characterizations and button cell fabrication. L.L. and Q.W. assisted in investigations and discussions on the Pr2−xBaxNiO4+δ defects and valence state change mechanism. F.X., M.K. and M.R.R. contributed to the in situ XRD characterizations. Z.S. performed part of the materials characterization and cell fabrication. Wenyuan Li provided suggestions on cell fabrication and electrochemical characterization and assisted in the acquisition of project funding. W.A.S. provided technical suggestions on the DFT and AIMD calculations. C.L. conducted part of the Raman spectroscopy characterizations. Xuemei Li assisted in the fabrication and electrochemical characterization of the nickel-based symmetric cells. Wei Li and H.T. wrote the original draft of the manuscript, response letter, revised manuscript and supplementary information. Y.-L.L. wrote the DFT and AIMD discussion in the original manuscript, response letter and revised manuscript. X. Liu reviewed and revised the paper. All authors discussed, commented and reviewed the paper.

Corresponding authors

Correspondence to Wei Li, Kai He or Xingbo Liu.

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Competing interests

H.T., Wenyuan Li and X. Liu have filed a patent application (US patent application no. 18/586661) on ‘Conformal coating scaffold electrodes for reversible solid oxide cells’. The other authors declare no competing interests.

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Nature Energy thanks Andrea Lanzini, Ryan O’Hayre, Emilia Olsson and Jose M. Serra for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Comparison of the fuel cell stability of the CCS-based PCECs in terms of degradation rates and operational duration with those of reported PCECs with the planar contact air electrode design.

The reported PCECs consist of various air electrodes/electrolytes combinations including BCFN/BHCYb (Ba0.9Co0.7Fe0.2Nb0.1O3−δ/BaHf0.1Ce0.7Yb0.2O3−δ), BCFZY/BZCYYb4411 (BaCo0.4Fe0.4Zr0.1Y0.1O3−δ/BaZr0.4Ce0.4Y0.1Yb0.1O3−δ), BCFN/BZCYYb1711 (Ba0.9Co0.7Fe0.2Nb0.1O3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), PBSLCC/BZCYYb1711 (Pr0.2Ba0.2Sr0.2La0.2Ca0.2CoO3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), PBCC/BNCYb (PrBa0.2Ca0.2Co2O5+δ/BaNb0.05Ce0.7Yb0.25O3–δ), PBCC/BTCYb (PrBa0.2Ca0.2Co2O5+δ/BaTa0.05Ce0.7Yb0.25O3–δ), SCFN/BZCYYb1711 (SrxCeyFemNinO3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), PBC-PCO/BZCYYb1711 (PrBaCo2O5+δ-Pr0.1Ce0.9O2+δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), LSCF-BCO/BZCYYb1711 (La0.6Sr0.4Co0.2Fe0.8O3–δ-BaCoO3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), BGPC-GCO/BZCYYb1711 (Ba0.8Gd0.8Pr0.4Co2O5+δ-GdxCoyO3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), PBCC/BMWCY (PrBa0.2Ca0.2Co2O5+δ/BaMo(W)0.03Ce0.71Yb0.26O3−δ), BCFZYN/BZCYYb1711 (Ba0.95(Co0.4Fe0.4Zr0.1Y0.1)0.95Ni0.05O3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), NCC/BZCYYb1711 (Na0.15Ca2.85Co4O9–δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ) (refs. 16,17,19,21,23,24,31,36,38,49,50,51). The FC stability and composition of the compared devices are detailed in Supplementary Table 4.

Source data

Extended Data Fig. 2 Comparison of the electrolysis cell stability of the CCS-based PCECs in terms of degradation rates and operational duration with those of reported PCECs with the planar contact air electrode design.

PBCC/BZCYYb1711 (PrBa0.2Ca0.2Co2O5+δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), GCCC/BZCYYb1711 (Gd0.3Ca2.7Co3.82Cu0.18O9−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ), LSCF-PBC-BCO/BZCYYb1711 ((La0.6Sr0.4)0.95Co0.2Fe0.8O3−δ-Pr1−xBaxCoO3−δ-BaCoO3−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ) (refs. 3,13,14,16,19,21,22,23,25,26,36,49,50,51). The EC stability and composition of the compared devices are detailed in Supplementary Table 5.

Source data

Extended Data Fig. 3 Comparison of the degradation rates of the CCS and DCS-based PCECs under different steam concentrations with those of reported PCECs with the planar-contact electrode design.

BCMN/BZCYYb1711 (Ba2Co1.5Mo0.25Nb0.25O6−δ/BaZr0.1Ce0.7Y0.1Yb0.1O3−δ) (refs. 3,6,13,14,16,17,19,21,22,23,24,25,26,31,36,38,49,50,51).

Source data

Extended Data Fig. 4 Simulated electrolysis polarization curves under different conditions at 600 °C.

a, Comparison of simulated electrolysis polarization curves of the PC and CCS electrodes with different grain particle diameters. The experimental polarization curve of CCS electrode with a grain diameter of 0.3–0.4 µm is shown for validation of the simulated one. b, Simulated electrolysis polarization curve of the CCS electrode as a function of relative hydration capability. c, Simulated electrolysis polarization curve of the CCS electrode as a function of relative proton diffusivity.

Source data

Supplementary information

Supplementary Information

Supplementary Methods, Figs. 1–97, Tables 1–18, Notes 1–18 and References.

Supplementary Video 1

The conduction of protons with and without the trapping effect of interstitial O was simulated using AIMD simulations. The two proton defects generated by the dissociated H2O in separated rock salt layers represent a proton adjacent to an interstitial O and a proton near an apical lattice O away from the interstitial O. The trajectories of these two protons are shown in the video.

Supplementary Video 2

The UR-PCEC prototype system was operated in EC mode at −1 A cm−2 for 12 h, representing the storage of electricity as H2 fuel at off-peak demand time, and then switched to the FC mode at 0.5 A cm−2 for 12 h, representing electricity generation using the stored H2 fuel at on-peak demand time. A typical 12/12 h cycle is shown in the video.

Supplementary Data 1

PBNO and PNO configurations for Supplementary Fig. 72, crystallographic information files for Supplementary Figs. 73 and 74c,d, Slab_figures_Ba_seg for Supplementary Fig. 75 and crystallographic configurations for Supplementary Figs. 83 and 85.

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Source Data Fig. 3

Source data for Fig. 3.

Source Data Fig. 4

Source data for Fig. 4c–f,h.

Source Data Fig. 5

Source data for Fig. 5c–h and inset of h.

Source Data Extended Data Fig. 1

Source data for Extended Data Fig. 1.

Source Data Extended Data Fig. 2

Source data for Extended Data Fig. 2.

Source Data Extended Data Fig. 3

Source data for Extended Data Fig. 3.

Source Data Extended Data Fig. 4

Source data for Extended Data Fig. 4.

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Tian, H., Li, W., Lee, YL. et al. Conformally coated scaffold design using water-tolerant Pr1.8Ba0.2NiO4.1 for protonic ceramic electrochemical cells with 5,000-h electrolysis stability. Nat Energy 10, 890–903 (2025). https://doi.org/10.1038/s41560-025-01800-1

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