Atomically dispersed platinum supported on curved carbon supports for efficient electrocatalytic hydrogen evolution

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Abstract

Dispersing catalytically active metals as single atoms on supports represents the ultimate in metal utilization efficiency and is increasingly being used as a strategy to design hydrogen evolution reaction (HER) electrocatalysts. Although platinum (Pt) is highly active for HER, given its high cost it is desirable to find ways to improve performance further while minimizing the Pt loading. Here, we use onion-like nanospheres of carbon (OLC) to anchor stable atomically dispersed Pt to act as a catalyst (Pt1/OLC) for the HER. In acidic media, the performance of the Pt1/OLC catalyst (0.27 wt% Pt) in terms of a low overpotential (38 mV at 10 mA cm−2) and high turnover frequencies (40.78 H2 s−1 at 100 mV) is better than that of a graphene-supported single-atom catalyst with a similar Pt loading, and comparable to a commercial Pt/C catalyst with 20 wt% Pt. First-principle calculations suggest that a tip-enhanced local electric field at the Pt site on the curved support promotes the reaction kinetics for hydrogen evolution.

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Fig. 1: Rational design of the Pt1/OLC catalyst via reducing the dimensions and introducing curvature.
Fig. 2: Structural identification of Pt single atom in Pt1/OLC catalyst.
Fig. 3: Hydrogen evolution performance of the Pt1/OLC catalyst.
Fig. 4: Theoretical investigation of the HER using the Pt1/OLC catalyst.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request

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Acknowledgements

This study was financially supported in part by the MOST (nos 2017YFA0303500 and 2018YFA0208603), the NSFC (nos 11574280, 11375198, U1532112, 91127042, 21790350, 21633006 and 21473166), the Recruitment Program of Global Experts and the CAS Hundred Talent Program and the Anhui Initiative in Quantum Information Technologies (AHY090200 and AHY090000). We thank the SSRF (14W1), the BSRF (1W1B and soft X-ray), the NSRL (photoemission, MCD and catalysis/surface science) and the USTC Center for Micro and Nanoscale Research and Fabrication for help with the characterization. We also thank Y. Liu and J. Shi for helpful discussions.

Author information

L.S. and J.J. conceived the research and designed the project. D.L. performed most of the experiments. X.L., S.D. and J.J. performed the simulations. S.C. contributed to the XAS measurements. H.Y. and J.L. contributed to the ALD preparation. B.G. contributed to the STEM characterizations. C. Wang, C. Wu and Y.A.H. partially contributed to experimental data. D.L., X.L., P.M.A., Y.L., J.J. and L.S. analysed the data and co-wrote the paper. All the authors discussed the results and commented on the manuscript.

Correspondence to Jun Jiang or Li Song.

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Supplementary Information

Supplementary Figs. 1–18, Supplementary Tables 1 and 2, and Supplementary references.

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