Research ArticleChemistry

Direct probing of atomically dispersed Ru species over multi-edged TiO2 for highly efficient photocatalytic hydrogen evolution

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Science Advances  23 Sep 2020:
Vol. 6, no. 39, eabb9823
DOI: 10.1126/sciadv.abb9823
  • Fig. 1 Schematic illustration of the synthetic procedure of ME-TiO2@Ru.

    Step I: Loading of the Ru component onto the surface of ME-PT. Step II: Pyrolysis of the Ru-loaded ME-PT for obtaining the final hybrid.

  • Fig. 2 Morphological, structural, and elemental characterizations.

    (A and B) FESEM images of Ru-loaded ME-PT. (C and D) TEM images of Ru-loaded ME-PT. (E and F) FESEM images of ME-TiO2@Ru. (G to I) TEM images of ME-TiO2@Ru. (J and K) HRTEM images of ME-TiO2@Ru. (L) HAADF-STEM image and related elemental mapping images of ME-TiO2@Ru; scale bar, 200 nm.

  • Fig. 3 EXAFS characterization.

    (A) Fourier-transformed magnitudes of the experimental Ru K-edge EXAFS spectra. (B and C) Fourier-transformed magnitudes of Ru K-edge EXAFS spectra in R space (B) and K space (C) for ME-TiO2@Ru. (D) Ru K-edge XANES experimental spectra. (E) WT for the k2-weighted EXAFS signal.

  • Fig. 4 H2 evolution and operando x-ray absorption spectroscopy.

    (A) Photocatalytic H2 generation rates of ME-TiO2@Ru with different Ru loading amounts. (B) Time-dependent hydrogen evolution over different catalysts. (C) Recycling tests (5 hours per cycle) of photocatalytic H2 generation of ME-TiO2@Ru. (D) Normalized operando Ru K-edge XANES spectra for ME-TiO2@Ru at various biases. (E and F) Ru K-edge EXAFS analysis of ME-TiO2@Ru in K (E) and R (F) spaces, respectively. The inset shows the structure of ME-TiO2@Ru under the reaction process. (G) Electron paramagnetic resonance spectra of ME-TiO2@Ru after different irradiation times. (H) Transient photocurrent spectra. (I) Time-resolved photoluminescence spectra. a.u., arbitrary units.

  • Fig. 5 DFT calculation.

    (A and B) Band structures of TiO2 (A) and Ru-decorated TiO2 (B). (C to E) Calculated density of states of TiO2 (C), TiO2@Ru (D), and ME-TiO2@Ru (E). (F to H) Calculated distribution of charge density (top) and differential charge density (bottom) for TiO2 (F), TiO2@Ru (G), and ME-TiO2@Ru (H).

Supplementary Materials

  • Supplementary Materials

    Direct probing of atomically dispersed Ru species over multi-edged TiO2 for highly efficient photocatalytic hydrogen evolution

    Huabin Zhang, Shouwei Zuo, Mei Qiu, Sibo Wang, Yongfan Zhang, Jing Zhang, Xiong Wen (David) Lou

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