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Stabilization of layered lithium-rich manganese oxide for anion exchange membrane fuel cells and water electrolysers

Nature Catalysis (2024)Cite this article

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Abstract

The design of materials that efficiently catalyse the electrochemical reaction of molecular oxygen to hydroxide ions is key to the development of electrochemical devices. Here we demonstrate an approach to control the orbital hybridization of 3d and 4d/5d metals to tune the adsorption strength and stabilize the catalytic sites in the platinum-free catalysts Li2Mn1−xRuxO3. We show that in these materials, the stabilization of O 2p holes by changing the M–O covalency (M = 4d/5d metal) can help to mitigate structural instability. Operando X-ray absorption spectroscopy revealed that the Mn and Ru atoms are the active sites for the oxygen reduction reaction (ORR) and exhibit a high ORR activity with noteworthy stability compared with the Pt/C catalyst and outperform NiFe layered double hydroxides and RuO2 in the oxygen evolution reaction. Notably, Li2Mn0.85Ru0.15O3 shows a high power density of 1.2 W cm−2 and current density of 1.2 A cm−2 at 1.9 V in the anion exchange membrane fuel cell and water electrolyser, respectively.

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Fig. 1: Physical characterization of the as-prepared Li2Mn1−xRuxO3 catalysts.
Fig. 2: Structural characterization of the as-prepared Li2Mn0.85Ru0.15O3.
Fig. 3: ORR activity and stability of Li2Mn1−xRuxO3.
Fig. 4: Operando XANES analysis and theoretical considerations.
Fig. 5: AEMFC performance using Li2Mn0.85Ru0.15O3 as cathode.
Fig. 6: OER performance using Li2Mn1−xRuxO3.

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Data availability

All of the data that support the findings of this study are available in the article. The atomic coordinates of the computational models developed in this study have been deposited at figshare at https://doi.org/10.6084/m9.figshare.25287826.v2 (ref. 70). Source data are provided with this paper.

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Acknowledgements

This work was funded by the National Natural Science Foundation of China (22179098, to J.M.). M.Y. acknowledges support from the National Natural Science Foundation of China (52302302), the Fundamental Research Funds for the Central Universities, the National Key R&D Program of China (2022YFE0208000) and HZWTECH for providing computational facilities. Z.H. acknowledges support from the Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials. P.S., T.K. and S.S. acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) through project number 403371556 GZ: INST 131/789-1 FUGG and the German–French Project ‘capital ReAlCharge’ (STR 596/13-1) and the German Federal Ministry of Education and Research (BMBF) through the HyThroughGen project within the technology platform ‘H2Giga’ (grant no. 03HY108D). P.S. and M.K. acknowledge the financial support by BMBF under grant numbers 03SF0613D ‘AEMready’, 03HY130B ‘AEM-Direkt’ and 03HY302Q ‘H2Mare’.

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Author notes

  1. Jin-Ming Chen

    Present address: Department of Electrophysics, National Yang Ming Chiao Tung University (NYCU), Hsinchu, Taiwan

  2. These authors contributed equally: Xuepeng Zhong, Lijun Sui, Menghao Yang.

Authors and Affiliations

  1. Shanghai Key Laboratory for R&D and Application of Metallic Functional Materials, Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai, China

    Xuepeng Zhong, Lijun Sui, Menghao Yang & Jiwei Ma

  2. Department of Chemistry, Technical University Berlin, Berlin, Germany

    Toshinari Koketsu, Malte Klingenhof & Peter Strasser

  3. Battery Materials Development Section, Business Creation Sector R&D Center, Mitsui Mining and Smelting Company, Limited, Saitama, Japan

    Toshinari Koketsu

  4. Center for Electron Microscopy (ZELMI), Technical University Berlin, Berlin, Germany

    Sören Selve

  5. Maison de la Simulation, CEA, CNRS, Université Paris-Sud, UVSQ, Université Paris-Saclay, Gif-sur-Yvette, France

    Kyle G. Reeves

  6. The Institute for Advanced Studies, Wuhan University, Wuhan, China

    Chuangxin Ge & Lin Zhuang

  7. Spallation Neutron Source Science Center, Dongguan, China

    Wang Hay Kan

  8. Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China

    Wang Hay Kan

  9. Australian Nuclear Science and Technology Organisation, Kirrawee DC, New South Wales, Australia

    Maxim Avdeev

  10. School of Chemistry, The University of Sydney, Sydney, Australia

    Maxim Avdeev

  11. Institute of Advanced Science Facilities, Shenzhen, China

    Miao Shu

  12. IC2MP, UMR-CNRS 7285, University of Poitiers, Poitiers, France

    Nicolas Alonso-Vante

  13. National Synchrotron Radiation Research Center, Hsinchu, Taiwan

    Jin-Ming Chen, Shu-Chih Haw, Chih-Wen Pao & Yu-Chung Chang

  14. State Key Laboratory of Material Processing and Die and Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, China

    Yunhui Huang

  15. Max Planck Institute for Chemical Physics of Solids, Dresden, Germany

    Zhiwei Hu

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Contributions

J.M. conceived the project and designed the experiments. X.Z., T.K., M.K., S.S., K.G.R., C.G., L.Z., W.H.K., M.A., M.S., N.A.-V., J.-M.C., S.-C.H., C.-W.P., Y.-C.C., Y.H., Z.H., P.S. and J.M. carried out the experimental work and data analysis. L.S. and M.Y. performed the theoretical calculations. All of the authors discussed the results and commented on the paper. X.Z., Z.H., P.S. and J.M. wrote the paper with contributions from all of the co-authors.

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Correspondence to Zhiwei Hu, Peter Strasser or Jiwei Ma.

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Zhong, X., Sui, L., Yang, M. et al. Stabilization of layered lithium-rich manganese oxide for anion exchange membrane fuel cells and water electrolysers. Nat Catal (2024). https://doi.org/10.1038/s41929-024-01136-1

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