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In-situ reconstructed Ru atom array on α-MnO2 with enhanced performance for acidic water oxidation

Nature Catalysis volume 4, pages 1012–1023 (2021)Cite this article

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Abstract

The development of acid-stable oxygen evolution reaction electrocatalysts is essential for high-performance water splitting. Here, we report an electrocatalyst with Ru-atom-array patches supported on α-MnO2 (Ru/MnO2) for the oxygen evolution reaction following a mechanism that involves only *O and *OH species as intermediates. This mechanism allows direct O–O radical coupling for O2 evolution. Ru/MnO2 shows high activity (161 mV at 10 mA cm−2) and outstanding stability with small degradation after 200 h operation, making it one of the best-performing acid-stable oxygen evolution reaction catalysts. Operando vibrational and mass spectroscopy measurements were performed to probe the reaction intermediates and gaseous products for validating the oxygen evolution reaction pathway. First-principles calculations confirmed the cooperative catalysis mechanism with a reduced energy barrier. Time-dependent elemental analysis demonstrated the occurrence of the in-situ dynamic cation exchange reaction during the oxygen evolution reaction, which is the key for triggering the reconstruction of Ru atoms into the ordered array with high durability.

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Fig. 1: Schematics of OER mechanisms for a heterogeneous Ru-based OER electrocatalyst.
Fig. 2: Structural characterization of the 12Ru/MnO2 catalyst.
Fig. 3: OER performance.
Fig. 4: OER process analysis.
Fig. 5: OER mechanism analysis based on DFT simulation results.
Fig. 6: OER mechanism analysis.

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Data availability

Source data are provided with this paper. The data supporting the findings of this study are available within the article and its Supplementary Information or from the corresponding authors upon reasonable request.

Code availability

The software codes for Large-scale Atomic Simulation with neural network Potential and the NN potentials used within the article are available from the corresponding authors upon request or on the website http://www.lasphub.com.

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Acknowledgements

J.-H.L. appreciates the support from the Creative Materials Discovery Program through the National Research Foundation of Korea funded by the Ministry of Science and ICT (2018M3D1A1057844). X.L. acknowledges financial support from the National Natural Science Foundation of China (no. 21972163), the Fundamental Research Funds for the Central Universities, the DHU Distinguished Young Professor Program, the Development Fund for Shanghai Talents, and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. Z.J. acknowledges the financial support from the National Natural Science Foundation of China (no. U1732267). XANES and EXAFS studies were carried out with the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (16ssrf00787). Z.-P.L. appreciates the support from National Key Research and Development Program of China (no. 2018YFA0208600). We thank Q. Liu from the University of Science and Technology of China for his helpful suggestions with synchrotron FTIR measurement and H. Zhang from the Shanghai Synchrotron Radiation Facility for his assistance in XPS analysis.

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  1. These authors contributed equally: Chao Lin, Ji-Li Li.

Authors and Affiliations

  1. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Songjiang District, Shanghai, P. R. China

    Chao Lin, Xiaopeng Li, Wei Luo & Yaojia Zhang

  2. Department of Materials Science and Chemical Engineering, Hanyang University, Ansan, Korea

    Chao Lin, Sung-Hae Kim, Dong-Hyung Kim, Sambhaji S. Shinde & Jung-Ho Lee

  3. Collaborative Innovation Center of Chemistry for Energy Material, Key Laboratory of Computational Physical Science (Ministry of Education), Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai, P. R. China

    Ji-Li Li, Ye-Fei Li & Zhi-Pan Liu

  4. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, P. R. China

    Shuai Yang & Zheng Jiang

  5. Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, P. R. China

    Zheng Jiang

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Contributions

C.L., X.L. and J.-H.L. conceived the project design. C.L. prepared the samples and measured their electrochemical properties. C.L., S.-H.K., D.-H.K. and S.S.S. performed the XPS, SEM and TEM characterizations. S.Y., Y.Z., X.L. and Z.J. performed the operando measurements and analysed the data. J.-L.L., Y.-F.L. and Z.-P.L. performed the DFT calculations. C.L., X.L., Z.J. and J.-H.L. wrote and revised the paper with help from all authors. W.L. helped with the manuscript revision. J.-H.L. supervised the research.

Corresponding authors

Correspondence to Xiaopeng Li, Zhi-Pan Liu, Zheng Jiang or Jung-Ho Lee.

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The authors declare no competing interests.

Additional information

Peer review information Nature Catalysis thanks Sergio Rojas, Kirsten Winther and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–34, Tables 1–13, Notes 1–7 and Methods.

Supplementary Data 1

The coordinates of structure by the fixed-cell SSW-NN method of Ru-doped MnO2 (110) surface in Supplementary Fig. 20.

Supplementary Data 2

The coordinates of structure for key intermediates of the LOM pathway on the Mn site in Supplementary Fig. 21.

Source data

Source Data Fig. 3

Chronopotentiometry curves.

Source Data Fig. 5

The coordinates of structures for key intermediates of the OPM and AEM reaction pathways.

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Lin, C., Li, JL., Li, X. et al. In-situ reconstructed Ru atom array on α-MnO2 with enhanced performance for acidic water oxidation. Nat Catal 4, 1012–1023 (2021). https://doi.org/10.1038/s41929-021-00703-0

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