Abstract
Rational design of noble metal catalysts with the potential to leverage efficiency is vital for industrial applications. Such an ultimate atom-utilization efficiency can be achieved when all noble metal atoms exclusively contribute to catalysis. Here, we demonstrate the fabrication of a wafer-size amorphous PtSex film on a SiO2 substate via a low-temperature amorphization strategy, which offers single-atom-layer Pt catalysts with high atom-utilization efficiency (~26 wt%). This amorphous PtSex (1.2 < x < 1.3) behaves as a fully activated surface, accessible to catalytic reactions, and features a nearly 100% current density relative to a pure Pt surface and reliable production of sustained high-flux hydrogen over a 2 inch wafer as a proof-of-concept. Furthermore, an electrolyser is demonstrated to generate a high current density of 1,000 mA cm−2. Such an amorphization strategy is potentially extendable to other noble metals, including the Pd, Ir, Os, Rh and Ru elements, demonstrating the universality of single-atom-layer catalysts.
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Data availability
The data that support the plots within this paper or other findings of this study are available from the corresponding authors on reasonable request, or included in the published article and its Supplementary Information. Source data are provided with this paper.
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Acknowledgements
This work was supported by the Singapore National Research Foundation Singapore programme (NRF-CRP21-2018-0007, NRF-CRP22-2019-0060, NRF-CRP18-2017-02 and NRF–CRP19–2017–01) and the Singapore Ministry of Education via AcRF Tier 3 (MOE2018-T3-1-002), AcRF Tier 2 (MOE2017-T2-2-136, MOE2019-T2-2-105 and MOE2018-T2-1-176) and AcRF Tier 1 (RG7/18 and 2019-T1-002-034). It was also supported by the National Key Research and Development Program of China (2019YFA0705400, 2021YFE0194200), the National Natural Science Foundation of China (11772153, 22073048, 21763024, 22175203, 22006023), the Natural Science Foundation of Jiangsu Province (BK20190018), the National Key R&D Program of China (2021YFA1500900), the Fundamental Research Funds for Central Universities (531119200209, NE2018002, NJ2020003) and the High-Performance Computing Center of Nanjing Tech University. Catalan Institute of Nanoscience and Nanotechnology (ICN2) acknowledges funding from Generalitat de Catalunya 2017SGR327 and the project NANOGEN (PID2020-116093RB-C43), funded by MCIN/AEI/10.13039/501100011033/. ICN2 is supported by the Severo Ochoa programme from Spanish MINECO (grant no. SEV-2017-0706) and is funded by the CERCA Programme/Generalitat de Catalunya. This work has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 823717-ESTEEM3. P.T. acknowledges Humboldt Research Fellowship for Postdoctoral Researchers sponsored by the Alexander von Humboldt Foundation. We thank S. Teddy (School of Materials Science and Engineering, Nanyang Technological University, Singapore) for XPS data analysis.
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Authors and Affiliations
Contributions
Z.L. and Y.H. conceived and initiated the project. Z.L. and Z. Zhang supervised the project and led the collaboration efforts. Y.H. designed the experiments, synthesized the PtSex films and performed the micro-/macro-electrochemical HER measurement. C.Z. (0000-0001-6383-3665), P.T., X.Z, M.H., R.E.D.-B. and J.A. performed the TEM, STEM and cross-sectional STEM measurements. Z. Zhang, L.L., W.G. and Z. Zhao performed atomistic computations and theoretical analyses. B.K. and B.S. did the electrolyser-cell measurements. P.G., S.G., M.X., C.Z. (0000-0002-1589-855X), X.W., L.Z., Z.S., C.G., J.Y. and H.D. assisted with the material characterizations, device fabrication and chemical vapour deposition synthesis. Y.D. conducted the XAS measurement. P.Y. helped with the synthesis of PtSe2 single crystal by the chemical vapour transport (CVT) method. Y.H., L.L., Q.J.W., Z. Zhang and Z.L. wrote the paper. All authors discussed the results and commented on the manuscript.
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Supplementary Information
Supplementary Figs. 1–50, Notes 1 and 2 and Tables 1–3.
Supplementary Video 1
Wafer-scale hydrogen production.
Supplementary Video 2
Electrolyser cell.
Source data
Source Data Fig. 2
The atomic coordinates of the optimized computational models in Fig. 2a.
Source Data Fig. 4
Time-dependent overpotential (ɳ) data under j = 20 mA cm−2 and 140 mA cm−2 in 0.5 M H2SO4 aqueous solution in Fig. 4b.
Source Data Fig. 5
The atomic coordinates of the optimized computational models in Fig. 5b.
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He, Y., Liu, L., Zhu, C. et al. Amorphizing noble metal chalcogenide catalysts at the single-layer limit towards hydrogen production. Nat Catal 5, 212–221 (2022). https://doi.org/10.1038/s41929-022-00753-y
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DOI: https://doi.org/10.1038/s41929-022-00753-y
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