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Rational design of Ru species on N-doped graphene promoting water dissociation for boosting hydrogen evolution reaction

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Abstract

In this study, the morphological distribution of Ru on nitrogen-doped graphene (NG) could be rationally regulated via modulating the combination mode between Ru precursor and the zeolite imidazolate framework-8 (ZIF-8). The cation exchange and host-guest strategies respectively resulted in two different combination modes between Ru precursor and ZIF-8 anchored on graphene. Following pyrolysis of the above precursors, Ru single-atom sites (SASs) with and without Ru nanoparticles (NPs) were formed selectively on NG (denoted as Ru SASs+NPs/NG and Ru SASs/NG, respectively). Ru SASs+NPs/NG exhibited excellent hydrogen evolution reaction (HER) performance in alkaline solutions (η10=12 mV, 12.57 A mg−1Ru at 100 mV), which is much better than Ru SASs/NG. The experimental and theoretical study revealed that Ru SASs could adsorb hydrogen with optimal adsorption strength, while Ru NPs could lower the barrier of water molecule dissociation, and thus Ru SASs and Ru NPs could synergistically promote the catalytic performance of HER in alkaline solutions.

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Acknowledgements

This work was supported by the National Key Research and Development Program of China (2020YFC1909604), Shenzhen Key Projects of Technological Research (JSGG20200925145800001), Shenzhen Basic Research Project (JCYJ20190808145203535, JCYJ20190808144413257), and the Project of Natural Science Foundation of Guangdong Province (2020A1515010379). We are grateful to the Instrumental Analysis Center of Shenzhen University (Xili Campus) for providing the facilities for our material analyzes and the Electron Microscopy Center at Shenzhen University for AC HAADF-STEM characterization. Thanks to Dr. Yantong Xu helped for DFT calculation.

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Authors and Affiliations

  1. Graphene Composite Research Center, Shenzhen University, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060, China

    Zhida Chen, Wenda Chen, Tao Huang, Jing Hu, Yaqi Lei, Qi Yuan, Xiangzhong Ren, Yongliang Li, Lei Zhang, Shenghua Ye, Qianling Zhang & Jianhong Liu

  2. Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9, Canada

    Xueliang Sun

  3. Shenzhen Eigen-Equation Graphene Technology Co. Ltd., Shenzhen, 518000, China

    Shaoluan Huang, Shenghua Ye & Jianhong Liu

  4. Institute of High Energy Physics Chinese Academy of Sciences, Beijing, 100049, China

    Lirong Zheng

  5. School of Materials Science and Engineering, Xiangtan University, Xiangtan, 411105, China

    Xiaoping Ouyang

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  1. Zhida Chen
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Correspondence to Shenghua Ye, Qianling Zhang, Xiaoping Ouyang, Xueliang Sun or Jianhong Liu.

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The authors declare no conflict of interest.

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The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Chen, Z., Chen, W., Zheng, L. et al. Rational design of Ru species on N-doped graphene promoting water dissociation for boosting hydrogen evolution reaction. Sci. China Chem. 65, 521–531 (2022). https://doi.org/10.1007/s11426-021-1163-7

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  • DOI: https://doi.org/10.1007/s11426-021-1163-7

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