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Heterogeneous synergistic catalysis by Ru-RuO x nanoparticles for Se–Se bond activation

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Abstract

The transition from homogeneous to heterogeneous synthetic chemistry enabled by nanocatalysts necessitates investigations of the reaction mechanism and structure-activity relationships for inorganic nanoparticles and organic substrates. Herein, we report that hydrothermally synthesized ruthenium nanoparticles performed differently in the Se–Se bond activation and selenylation of heterocycles, exhibiting a volcano-shaped relationship between catalytic activity and composition. A synergistic effect was observed for Ru-RuO x nanocatalysts, with numerous characterizations and density functional theory (DFT) calculations suggesting that a PhSeSePh molecule can initially be adsorbed on the metallic Ru sites and cleaved into two PhSe* species, which subsequently migrate to RuO x sites and react with the nucleophile to achieve the selenylation of heterocycles.

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Acknowledgements

We thank the National Natural Science Foundation of China (Nos. 21461162001, 21025101, 21371011, 21321001, 21229101, and 21331001), the National Basic Research Program of China (No. 2012CBA01204) for financial support, and the 7th China Postdoctoral Science Foundation Funded Project (No. 2014T70009). M. L. was also supported in part by the Postdoctoral Fellowship of Peking-Tsinghua Center for Life Sciences.

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China

    Mu Lin, Liqun Kang, Jun Gu, Linxiu Dai, Shengbo Tang, Tao Zhang, Yuhao Wang, Lindong Li, Xiaoyu Zheng, Wei Zhu, Xuefeng Fu, Lingdong Sun, Yawen Zhang & Chunhua Yan

  2. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China

    Rui Si

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  1. Mu Lin
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Correspondence to Lingdong Sun, Yawen Zhang or Chunhua Yan.

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Lin, M., Kang, L., Gu, J. et al. Heterogeneous synergistic catalysis by Ru-RuO x nanoparticles for Se–Se bond activation. Nano Res. 10, 922–932 (2017). https://doi.org/10.1007/s12274-016-1350-0

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  • DOI: https://doi.org/10.1007/s12274-016-1350-0

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