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Sub-nm ruthenium cluster as an efficient and robust catalyst for decomposition and synthesis of ammonia: Break the “size shackles”

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Abstract

Downsizing to sub-nm is a general strategy to reduce the cost of catalysts. However, theoretical Wulff-constructed model suggests that sub-nm clusters show little activity for various reactions such as ammonia decomposition and ammonia synthesis because of the lack of active sites. As clusters may deviate from the ideal model construction under reaction conditions, a host–guest strategy to synthesize thermally stable 1.0 nm monodispersed Ru clusters by the pyrolysis of MIL-101 hosts is reported here to verify the hypothesis. For ammonia decomposition, the activity of the Ru clusters is 25 times higher than that of commercial Ru/active carbon (AC) at full-conversion temperature, while for ammonia synthesis, the activity of the Ru clusters is 500 times as high as that of promoted Ru NPs counterpart. The catalyst also maintains its activities for 40 h without any increase in the size. This model can be used to develop a host–guest strategy for designing thermally stable sub-nm clusters to atomic–efficiently catalyze reactions.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21521091, 21131004, 21390393, U1463202, 21573119, 21590792, and 21406184). We also thank the Shanghai Synchrotron Radiation Facility (No. BL14W1) for providing beam time.

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  1. Jinpeng Li and Weiyang Wang contributed equally to this work.

Authors and Affiliations

  1. Department of Chemistry, Tsinghua University, Beijing, 100084, China

    Jinpeng Li, Weiyang Wang, Wenxing Chen, Dingsheng Wang, Qing Peng, Wei Zhu, Chen Chen & Yadong Li

  2. The Center of New Energy Materials and Technology, College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu, 610500, China

    Qinmei Gong & Hui Zhang

  3. Center for Electron Microscopy, Tianjin University of Technology, Tianjin, 300384, China

    Jun Luo

  4. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York, 11973, USA

    Ruoqian Lin & Huolin Xin

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  1. Jinpeng Li
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Correspondence to Wei Zhu or Chen Chen.

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Sub-nm ruthenium cluster as an efficient and robust catalyst for decomposition and synthesis of ammonia: Break the “size shackles”

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Li, J., Wang, W., Chen, W. et al. Sub-nm ruthenium cluster as an efficient and robust catalyst for decomposition and synthesis of ammonia: Break the “size shackles”. Nano Res. 11, 4774–4785 (2018). https://doi.org/10.1007/s12274-018-2062-4

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