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Reversed Charge Transfer and Enhanced Hydrogen Spillover in Platinum Nanoclusters Anchored on Titanium Oxide with Rich Oxygen Vacancies Boost Hydrogen Evolution Reaction
Author(s) -
Wei ZhenWei,
Wang HongJuan,
Zhang Chao,
Xu Kun,
Lu XiuLi,
Lu TongBu
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202104856
Subject(s) - nanoclusters , hydrogen spillover , catalysis , platinum , hydrogen , electron transfer , oxygen , chemistry , oxide , titanium , inorganic chemistry , materials science , photochemistry , nanotechnology , organic chemistry
The catalytic activity of metal clusters is closely related with the support; however, knowledge on the influence of the support on the catalytic activity is scarce. We demonstrate that Pt nanoclusters (NCs) anchored on porous TiO 2 nanosheets with rich oxygen vacancies ( V O ‐rich Pt/TiO 2 ) and deficient oxygen vacancies ( V O ‐deficient Pt/TiO 2 ), display significantly different catalytic activity for the hydrogen evolution reaction (HER), in which V O ‐rich Pt/TiO 2 shows a mass activity of 45.28 A mg Pt −1 at −0.1 V vs. RHE, which is 16.7 and 58.8 times higher than those of V O ‐deficient Pt/TiO 2 and commercial Pt/C, respectively. DFT calculations and in situ Raman spectra suggest that porous TiO 2 with rich oxygen vacancies can simultaneously achieve reversed charge transfer (electrons transfer from TiO 2 to Pt NCs) and enhanced hydrogen spillover from Pt NCs to the TiO 2 support, which leads to electron‐rich Pt NCs being amenable to proton reduction of absorbed H*, as well as the acceleration of hydrogen desorption at Pt catalytic sites—both promoting the HER. Our work provides a new strategy for rational design of highly efficient HER catalysts.