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Abrading bulk metal into single atoms

Nature Nanotechnology volume 17, pages 403–407 (2022)Cite this article

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Abstract

Single-atom catalysts have recently attracted considerable attention because of their highly efficient metal utilization and unique properties. Finding a green, facile method to synthesize them is key to their widespread commercialization. Here we show that single-atom catalysts (including iron, cobalt, nickel and copper) can be prepared via a top-down abrasion method, in which the bulk metal is directly atomized onto different supports, such as carbon frameworks, oxides and nitrides. The level of metal loading can be easily tuned by changing the abrasion rate. No synthetic chemicals, solvents or even water were used in the process and no by-products or waste were generated. The underlying reaction mechanism involves the mechanochemical force in situ generating defects on the supports, then trapping and stably sequestering atomized metals.

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Fig. 1: Schematic comparing the different methods for preparing SACs.
Fig. 2: Characterizations of single-atom metal–N–C.
Fig. 3: Theoretical analysis.
Fig. 4: Extension to different supports.

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Data availability

The data that support the findings of this study are presented in the main text and the Supplementary Information, and are available from the corresponding authors upon reasonable request.

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Acknowledgements

We thank M. Chhowalla for help and discussion. We are grateful for the use of the Pohang Accelerator Laboratory (6D UNIST-PAL beamline, South Korea). J.-B.B. acknowledges support from the Creative Research Initiative (CRI, 2014R1A3A2069102) and Science Research Center (SRC, 2016R1A5A1009405) programmes through the National Research Foundation (NRF) of Korea. J.-B.B also acknowledges the U-K Brand Project (1.200096.01) of UNIST. H.Y.J. acknowledges support from the National R&D Program (2020M3F3A2A01082618) through the National Research Foundation (NRF) of Korea. F.L. acknowledges financial support from Fudan University (JIH2203011). Funding for J.W., A.I.R., W.Z. and R.G. was provided by the International Partnership Program of the Chinese Academy of Sciences (121421KYSB20170020) and the State Key Laboratory of Catalysis in Dalian Institute of Chemical Physics (N-16-07). Z.A. acknowledges financial support (221777033) from the National Natural Science Foundation of China.

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Authors and Affiliations

  1. School of Energy and Chemical Engineering/Center for Dimension-Controllable Organic Frameworks, Ulsan National Institute of Science and Technology (UNIST), Ulsan, South Korea

    Gao-Feng Han, Feng Li, Yoon-Kwang Im, Soo-Young Yu, Jong-Pil Jeon, Seok-Jin Kim & Jong-Beom Baek

  2. Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, P. R. China

    Feng Li

  3. Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, P. R. China

    Alexandre I. Rykov, Wenhui Zhou, Rile Ge & Junhu Wang

  4. Institute of Environmental Health and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, P. R. China

    Zhimin Ao

  5. Graduate School of Semiconductor Materials and Devices Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, South Korea

    Tae Joo Shin & Hu Young Jeong

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  1. Gao-Feng Han
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Contributions

J.-B.B. conceived the project and oversaw all the research phases. J.-B.B. and G.-F.H. designed the project. G.-F.H. carried out the sample synthesis and structural characterization. F.L. and Z.A. performed the DFT calculation. T.J.S., Y.-K.I., J.-P.J. and S.-J.K. assisted with the XAS study. H.Y.J. conducted the HAADF-STEM measurements. J.W., A.I.R., W.Z. and R.G. measured and interpreted the Mössbauer spectroscopy. S.-Y.Y. designed the scheme. Data collection and analysis were conducted by J.-B.B., G.-F.H. and F.L. All the authors contributed to the writing of the manuscript.

Corresponding authors

Correspondence to Feng Li, Hu Young Jeong or Jong-Beom Baek.

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Nature Nanotechnology thanks the anonymous reviewers for their contribution to the peer review of this work.

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Supplementary methods, notes, Figs. 1–15 and Tables 1–5.

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Han, GF., Li, F., Rykov, A.I. et al. Abrading bulk metal into single atoms. Nat. Nanotechnol. 17, 403–407 (2022). https://doi.org/10.1038/s41565-022-01075-7

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