4.6 Article

Surface oxygen vacancies promoted Pt redispersion to single-atoms for enhanced photocatalytic hydrogen evolution

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 9, Issue 24, Pages 13890-13897

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta01400e

Keywords

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Funding

  1. National Natural Science Foundation of China [21905253, 51973200, 92061201, 21825106]
  2. China Postdoctoral Science Foundation [2018M640681, 2019T120632, 2020M682332]
  3. Henan Postdoctoral Foundation [202003015]
  4. Program for Innovative Research Team (in Science and Technology) in Universities of Henan Province [19IRTSTHN022]

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Utilizing the hydrogen spillover effect at high temperature, surface oxygen vacancies on TiO2 can facilitate the redispersion of Pt nanoparticles to stable single-atoms, leading to excellent photocatalytic water splitting performance. This approach provides a facile method to prepare noble metal catalysts with both high atom economy and reaction activity.
Isolating metal atoms on supports for catalysis has attracted great attention of researchers due to the unique catalytic properties. Here we show by utilizing the hydrogen spillover effect at high temperature (700 degrees C) that the in situ formed surface oxygen vacancies on TiO2 nanobelts can facilitate the redispersion of Pt nanoparticles to stable single-atoms. The isolated Pt atoms are firmly confined by the surface oxygen vacancy sites in the internal surface of TiO2. Density functional theory (DFT) calculations have further proved that Pt atom is likely to be confined to oxygen vacancies to form single-atom sites. The as-obtained catalyst exhibits excellent photocatalytic water splitting performance with a hydrogen evolution rate of 38.33 mmol mg(Pt)(-1) h(-1) under simulated solar light irradiation, which is about 59.9 times higher than that of TiO2 nanobelts with Pt nanoparticles. This approach provides a facile method to prepare noble metal catalysts with both high atom economy and reaction activity.

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