期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 17, 页码 5719-5727出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b13736
关键词
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资金
- National Key Research and Development Program of China [2016YFB0901600]
- National Science Foundation of China [51402334, 51502331]
- Science and Technology Commission of Shanghai [14520722000]
- Key Research Program of Chinese Academy of Sciences [KGZD-EW-T06]
- National Natural Science Foundation of China [51572016, U1530401]
- Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund [U1501501]
TiO2 mesoporous crystal has been prepared by one-step corroding process via an oriented attachment (OA) mechanism with SrTiO3 as precursor. High resolution transmission electron microscopy (HRTEM) and nitrogen adsorption desorption isotherms confirm its mesoporous crystal structure. Well-dispersed ruthenium (Ru) in the mesoporous nanocrystal TiO2 can be attained by the same process using Ru-doped precursor SrTi1-xRuxO3. Ru is doped into lattice of TiO2, which is identified by HRTEM and super energy dispersive spectrometer (super-EDS) elemental mapping. X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance spectroscopy (EPR) suggest the pentavalent Ru but not tetravalent, while partial Ti in TiO2 accept an electron from Ru and become Ti3+, which is observed for the first time. This Ru-doped TiO2 performs high activity for electrocatalytic hydrogen evolution reaction (HER) in alkaline solution. First principles calculations simulate the HER process and prove TiO2:Ru with Ru5+ and Ti3+ holds high HER activity with appropriate hydrogen-adsorption Gibbs free energies (Delta G(H)).
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