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High temperature shockwave stabilized single atoms

Nature Nanotechnology volume 14, pages 851–857 (2019)Cite this article

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Abstract

The stability of single-atom catalysts is critical for their practical applications. Although a high temperature can promote the bond formation between metal atoms and the substrate with an enhanced stability, it often causes atom agglomeration and is incompatible with many temperature-sensitive substrates. Here, we report using controllable high-temperature shockwaves to synthesize and stabilize single atoms at very high temperatures (1,500–2,000 K), achieved by a periodic on–off heating that features a short on state (55 ms) and a ten-times longer off state. The high temperature provides the activation energy for atom dispersion by forming thermodynamically favourable metal–defect bonds and the off-state critically ensures the overall stability, especially for the substrate. The resultant high-temperature single atoms exhibit a superior thermal stability as durable catalysts. The reported shockwave method is facile, ultrafast and universal (for example, Pt, Ru and Co single atoms, and carbon, C3N4 and TiO2 substrates), which opens a general route for single-atom manufacturing that is conventionally challenging.

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Fig. 1: In situ high-temperature-shockwave synthesis of HT-SAs on defective carbon.
Fig. 2: Thermal stability of the HT-SAs.
Fig. 3: HT-SA dispersion mechanism and temperature effect
Fig. 4: The generality of the shockwave method and HT-SAs in catalytic reactions.

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Data availability

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

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Acknowledgements

This project is not directly funded. We acknowledge the support of the Maryland Nanocenter, its Surface Analysis Center and AIMLab and the University of Maryland supercomputing resources (http://hpcc.umd.edu). Z.H. and R.S.-Y. acknowledge the financial support from NSF-DMR award no. 1809439. P.X. and Chao Wang thank the support from the Advanced Research Projects Agency—Energy (ARPA-E), Department of Energy (DOE) and the Petroleum Research Fund, American Chemical Society. L.M., T.W. and J.L. acknowledge the financial support from the US Department of Energy under Contract DE-AC02-06CH11357. Research conducted at beamline 9-BM used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US DOE by Argonne National Laboratory under Contract no. DE-AC02-06CH11357. Chongmin Wang thanks the support of LDRD of PNNL and the in situ ETEM was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE’s Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the Department of Energy under Contract DE-AC05-76RLO1830.

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Author notes

  1. These authors contributed equally: Yonggang Yao, Zhennan Huang, Pengfei Xie, Lianping Wu, Lu Ma, Tangyuan Li

Authors and Affiliations

  1. Department of Materials Science and Engineering, University of Maryland, College Park, MD, USA

    Yonggang Yao, Tangyuan Li, Miaolun Jiao, Zhiqiang Liang, Jinlong Gao & Liangbing Hu

  2. Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, IL, USA

    Zhennan Huang & Reza Shahbazian-Yassar

  3. Department of Chemical and Biomolecular Engineering, Johns Hopkins University, Baltimore, MD, USA

    Pengfei Xie & Chao Wang

  4. Department of Mechanical Engineering, University of Maryland, College Park, MD, USA

    Lianping Wu, Zhenqian Pang & Teng Li

  5. X-ray Science Division and Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA

    Lu Ma, Jun Lu & Tianpin Wu

  6. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USA

    Yang He & Chongmin Wang

  7. Department of Chemical and Biomolecular Engineering and Chemistry and Biochemistry, University of Maryland, College Park, MD, USA

    Dylan Jacob Kline & Michael R. Zachariah

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  1. Yonggang Yao
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Contributions

L.H. and Y.Y. contributed to the idea and experimental design. Y.Y., T.L., M.J. and Z.L. conducted the experiments and materials preparation. Z.H. and R.S.-Y. performed the high-resolution microscopy. P.X. and Chao Wang contributed to the catalysis evaluation. L.W., Z.P. and T.L. conducted the simulation analysis. L.M., T.W. and J.L. contributed to the X-ray absorption measurements and analysis. Y.H. and Chongmin Wang performed the in situ environmental microscopy. D.J.K. and M.R.Z. performed the temperature characterization and thermal gravimetric analysis. L.H. and Y.Y. wrote the paper and all the authors commented on the final manuscript.

Corresponding authors

Correspondence to Tianpin Wu, Teng Li, Chao Wang, Reza Shahbazian-Yassar or Liangbing Hu.

Additional information

Peer review information: Nature Nanotechnology thanks Abhaya (Krishna) Datye, Frédéric Jaouen and Yadong Li for their contribution to the peer review of this work.

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Yao, Y., Huang, Z., Xie, P. et al. High temperature shockwave stabilized single atoms. Nat. Nanotechnol. 14, 851–857 (2019). https://doi.org/10.1038/s41565-019-0518-7

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