Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 30, Pages 16622-16627Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202104856
Keywords
charge transfer reversion; electrocatalysis; hydrogen spillover effect; platinum nanoclusters
Categories
Funding
- National Key R&D Program of China [2017YFA0700104]
- National Natural Science Foundation of China [21790052, 21805207, 21931007]
- 111 Project of China [D17003]
- Science & Technology Development Fund of Tianjin Education Commission for Higher Education [2018KJ129]
Ask authors/readers for more resources
The study demonstrates that Pt nanoclusters supported on porous TiO2 nanosheets with rich oxygen vacancies exhibit significantly higher catalytic activity for the HER compared to those supported on TiO2 with deficient oxygen vacancies. This is attributed to the ability of the TiO2 support with rich oxygen vacancies to facilitate reversed charge transfer and enhanced hydrogen spillover, promoting proton reduction and hydrogen desorption at Pt catalytic sites. This work provides a new strategy for the rational design of highly efficient HER catalysts.
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 TiO2 nanosheets with rich oxygen vacancies (V-O-rich Pt/TiO2) and deficient oxygen vacancies (V-O-deficient Pt/TiO2), display significantly different catalytic activity for the hydrogen evolution reaction (HER), in which V-O-rich Pt/TiO2 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/TiO2 and commercial Pt/C, respectively. DFT calculations and in situ Raman spectra suggest that porous TiO2 with rich oxygen vacancies can simultaneously achieve reversed charge transfer (electrons transfer from TiO2 to Pt NCs) and enhanced hydrogen spillover from Pt NCs to the TiO2 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.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available