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Rational design of perovskite ferrites as high-performance proton-conducting fuel cell cathodes

Nature Catalysis volume 5, pages 777–787 (2022)Cite this article

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Abstract

The biggest obstacle to the commercialization of protonic ceramic fuel cells (PCFCs) is the lack of high-performance, low-cost cathode materials. Currently, the most promising cathode materials are cobalt-based perovskites; however, the unstable phases, poor thermomechanical compatibility with other PCFC components, high cost and unsatisfactory performance limit the viability of these materials. Here we combine ab initio simulations, molecular orbital insights, and A- and B-site co-substitution to develop a cobalt-free perovskite with outstanding performance. A- and B-site substitution in BaFeO3−δ, is found to promote the formation of oxygen vacancies (\({{{\mathrm{V}}}}_{{{\mathrm{O}}}}^{ \bullet \bullet }\)) and hydroxyl ions (\({{{\mathrm{OH}}}}_{{{\mathrm{O}}}}^ \bullet\)) while retaining structural stability. The best computationally identified material, Ba0.875Fe0.875Zr0.125O3−δ, showed exceptional oxygen reduction reaction electrochemical activity with a peak power density of 0.67 W cm−2 at 500 °C. This rational approach provides a strategy for designing high-activity, low-cost and cobalt-free perovskites, marking a significant step towards realizing commercially viable PCFCs.

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Fig. 1: DFT-calculated Eform, \({{E}}_{{{{\mathrm{vac}}}}}\left( {{{{\mathrm{V}}}}_{{{\mathrm{O}}}}^{ \bullet \bullet }} \right)\) and Ehydr.
Fig. 2: Contour plot of BFO and derivative materials.
Fig. 3: Metal–oxygen bond molecular orbital interactions and PDOS analyses.
Fig. 4: Schematic illustration of the two chemical environments of \({{{\mathrm{V}}}}_{{{\mathrm{O}}}}^{ \bullet \bullet }\) and \({{{\mathrm{OH}}}}_{{{\mathrm{O}}}}^ \bullet\).
Fig. 5: DFT calculations of the ORR on D-BFZ.
Fig. 6: Structural characterization by X-ray diffraction, XPS, TEM and XANES.
Fig. 7: Hydrogen permeation test, SEM characterization and fuel cell test of D-BFZ.

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Data availability

The data that support the findings of this study are available within the article and its Supplementary Information files or from the corresponding author upon reasonable request. The atomic coordinates of the optimized structures are provided in Supplementary Data 1. Source data are provided with this paper.

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Acknowledgements

The authors gratefully acknowledge the Research Grant Council of Hong Kong for support through the projects (16201820 and 16206019, received by F.C.), the Nano & Material Technology Development Project (NRF-2021M3H4A1A01002919, received by F.C.) and the Global PhD Fellowship through the National Research Foundation (NRF) of Korea, funded by the Ministry of Science, ICT, and Future Planning (NRF-2018H1A2A1060644, received by A.S.). This work was supported in part by the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone (HZQB-KCZYB-2020083, received by F.C.). M.J.R. and A.B. kindly recognize the support of the Hong Kong PhD Fellowship Scheme. We are grateful to the Materials Characterization and Preparation Facility (MCPF) and the Advanced Engineering Materials Facility (AEMF) of the Hong Kong University of Science and Technology for their assistance in experimental characterizations. The calculations were performed on the Tianhe-2 supercomputer system in Guangzhou.

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  1. These authors contributed equally: Zheng Wang, Yuhao Wang, Jian Wang, Yufei Song.

Authors and Affiliations

  1. Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, China

    Zheng Wang, Yuhao Wang, Yufei Song, Matthew J. Robson, Zhiqi Zhang, Alessio Belotti, Jiapeng Liu & Francesco Ciucci

  2. School of Energy and Environment, City University of Hong Kong, Hong Kong, China

    Jian Wang

  3. Department of Chemistry, College of Science, Seoul National University, Seoul, South Korea

    Jian Wang & Jongwoo Lim

  4. Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology, Ulsan, South Korea

    Arim Seong & Guntae Kim

  5. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, China

    Meiting Yang & Zongping Shao

  6. Department of Chemical Engineering, Curtin University, Perth, Western Australia, Australia

    Zongping Shao

  7. HKUST Shenzhen–Hong Kong Collaborative Innovation Research Institute, Shenzhen, China

    Francesco Ciucci

  8. Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong, China

    Francesco Ciucci

  9. Energy Institute, The Hong Kong University of Science and Technology, Hong Kong, China

    Francesco Ciucci

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Contributions

Z.W., Y.W. and F.C. conceived and designed the project. Z.W. performed theoretical calculations. Y.W. fabricated fuel cells and performed X-ray diffraction and SEM analyses. Y.S., M.Y., A.S., G.K. and Z.S. measured proton conductivity. J.W. and J.Lim performed X-ray absorption spectroscopy characterizations and contributed to data analysis. Z.Z., A.B. and J.Liu performed TEM characterizations. Z.W., Y.W., Y.S., M.J.R. and F.C. drafted the manuscript. All authors reviewed the manuscript.

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Correspondence to Francesco Ciucci.

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Nature Catalysis thanks Chuancheng Duan, Kevin Huang and Ivano Castelli for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–42, Tables 1–12, methods and references.

Supplementary Data

Contains the coordinates of the calculated species in this article.

Source data

Source Data Fig. 1

Contains the energies of calculated species.

Source Data Fig. 2

Contains the energies of calculated species.

Source Data Fig. 3

The projected density of state of Fe–O, Zr–O and Y–O bonds

Source Data Fig. 5

Contains the energies of calculated intermediates of oxygen reduction reactions for BFZ, BFZ-1Vo, BFZ-2Vo and BFZ-2Vo-2OHo

Source Data Fig. 6

The data used to plot the figures.

Source Data Fig. 7

The data used to plot the figures.

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Wang, Z., Wang, Y., Wang, J. et al. Rational design of perovskite ferrites as high-performance proton-conducting fuel cell cathodes. Nat Catal 5, 777–787 (2022). https://doi.org/10.1038/s41929-022-00829-9

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