4.7 Article

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

Journal

SCIENCE CHINA-CHEMISTRY
Volume 65, Issue 3, Pages 521-531

Publisher

SCIENCE PRESS
DOI: 10.1007/s11426-021-1163-7

Keywords

Ru; single atomic sites; nanoparticles; water dissociation; synergistic effect

Funding

  1. National Key Research and Development Program of China [2020YFC1909604]
  2. Shenzhen Key Projects of Technological Research [JSGG20200925145800001]
  3. Shenzhen Basic Research Project [JCYJ20190808145203535, JCYJ20190808144413257]
  4. Project of Natural Science Foundation of Guangdong Province [2020A1515010379]

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The morphological distribution of Ru on nitrogen-doped graphene can be regulated by modulating the combination mode. In alkaline solutions, the combination of Ru single-atom sites and Ru nanoparticles can synergistically promote excellent hydrogen evolution reaction performance.
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 (eta(10)=12 mV, 12.57 A mg(Ru)(-1) 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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