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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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.
Change history
26 April 2024
A Correction to this paper has been published: https://doi.org/10.1038/s41929-024-01166-9
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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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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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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 7, 546–559 (2024). https://doi.org/10.1038/s41929-024-01136-1
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DOI: https://doi.org/10.1038/s41929-024-01136-1
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