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Gas-balancing adsorption strategy towards noble-metal-based nanowire electrocatalysts

Nature Catalysis volume 7, pages 719–732 (2024)Cite this article

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Abstract

The preparation of noble metal nanowire electrocatalysts is greatly limited by the thermodynamically symmetric growth of face-centred-cubic structures. Here we report a gas-balancing adsorption strategy to prepare ultrathin palladium-, platinum- and gold-based nanowires (diameter < 2 nm) by controlling the competitive adsorption of in situ-generated H2 and CO. We prepare a library of 43 nanowires consisting of the three above-mentioned noble metals as hosts and 14 metals as guests. The ternary Pd85Pt8Ni7H41 nanowires with interstitial hydrogen exhibit impressive mass and specific activities of \(11.1 \, {\rm{A}}\,{\rm{mg}}_{{\rm{PGM}}}^{-1}\) and 13.9 mA cm−2, respectively, for the oxygen reduction reaction at 0.9 VRHE in alkali. Operando X-ray absorption spectroscopy demonstrates breathing-like Pd–Pd bond length and strain changes at the applied potential, with Pd85Pt8Ni7H41 nanowires exhibiting larger compressive strain at relevant potentials, as well as low oxygen coverage. Theoretical calculations suggest that the interstitial hydrogen induces an s–d orbital interaction between palladium and hydrogen, which enhances the activity of the oxygen reduction reaction. The Pd85Pt8Ni7H41 nanowires can generate a high power density of 0.87 W cm−2 in H2/air (CO2-free) at 70 °C in an anion-exchange membrane fuel cell.

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Fig. 1: Morphology characterizations of Pd-based nanowires.
Fig. 2: Morphology characterizations of Pt- and Au-based nanowires.
Fig. 3: Summary and formation mechanism of Pt-, Pd- and Au-based NWs libraries.
Fig. 4: Structural characterizations of PdHx-based NWs.
Fig. 5: Electrochemical tests of the Pd-based NWs in 0.1 M KOH.
Fig. 6: Mechanism investigations of the enhanced ORR activity of PdHx-based NWs.
Fig. 7: MEA performance of Pd- and Pt-based NWs.

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The data that support the findings of this study are available from the corresponding author upon reasonable request. Source Data are provided with this paper.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (grant no. 22122202 to Q.L.), National Key Research and Development Program of China (grant nos. 2021YFA1501001 and 2021YFA1600800, Q.L.) and NSF-PREM program (grant no. DMR-1828019 to G.L.). We thank the Analytical and Testing Center of the Huazhong University of Science and Technology (HUST) for performing the TEM and XRD measurements, and the BL11B beamline in the Shanghai Synchrotron Radiation Facility (SSRF) for providing the beam time. This work is supported by the Pico Center at SUSTech CRF which receives support from the Presidential Fund and Development and Reform Commission of Shenzhen Municipality.

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Author notes

  1. These authors contributed equally: Jiashun Liang, Shenzhou Li, Xuan Liu.

Authors and Affiliations

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

    Jiashun Liang, Shenzhou Li, Xuan Liu, Hao Shi, Siyang Zhang, Yunhui Huang & Qing Li

  2. Institute for Advanced Materials, School of Materials Science and Engineering, Jiangsu University, Zhenjiang, China

    Yangyang Wan

  3. Department of Physics and Astronomy, California State University Northridge, Northridge, CA, US

    Yangyang Wan & Gang Lu

  4. Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, China

    Yu Xia & Hsing-Lin Wang

  5. School of Physics and Astronomy, University of Birmingham, Birmingham, UK

    Yu Xia

  6. Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, US

    Gang Wu

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  1. Jiashun Liang
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Contributions

Q.L. and J.L. conceived the idea and designed the experiments. J.L., X.L, S.L., H.S. and S.Z. performed the sample synthesis, characterization and electrochemical measurements. Y.X., and H.-L.W. performed HAADF-STEM characterizations. Y.W. and G.L. provided theoretical calculations. J.L., Q.L., G.W. and Y.H. wrote and revised the paper. All of the authors contributed to the overall scientific discussion and edited the paper.

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Correspondence to Qing Li.

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Nature Catalysis thanks Sang-Il Choi, Alessandro Long, Xueqiang Qi and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–76, Tables 1–11 and Notes 1–8.

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CIF data of the computational models.

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CIF data of the computational models.

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CIF data of the computational models.

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Liang, J., Li, S., Liu, X. et al. Gas-balancing adsorption strategy towards noble-metal-based nanowire electrocatalysts. Nat Catal 7, 719–732 (2024). https://doi.org/10.1038/s41929-024-01167-8

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