Journal
NANO LETTERS
Volume 18, Issue 6, Pages 3785-3791Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b01059
Keywords
Platinum; nickel; single atoms; selective hydrogenation; hydrogen diffusion
Categories
Funding
- Collaborative Innovation Center of Suzhou Nano Science and Technology
- MOST of China [2014CB932700]
- NSFC [21573206, 51601186, 21473167, 21421063]
- CAS [QYZDB-SSW-SLH017, XDA09030102]
- Hundred Talents project of the CAS
- Anhui Provincial Key Scientific and Technological Project [1704a0902013]
- Major Program of Development Foundation of Hefei Center for Physical Science and Technology [2017FXZY002]
- Fundamental Research Funds for the Central Universities
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Single-atom catalysts exhibit high selectivity in hydrogenation due to their isolated active sites, which ensure uniform adsorption configurations of substrate molecules. Compared with the achievement in catalytic selectivity, there is still a long way to go in exploiting the catalytic activity of single-atom catalysts. Herein, we developed highly active and selective catalysts in selective hydrogenation by embedding Pt single atoms in the surface of Ni nanocrystals (denoted as Pt-1/Ni nanocrystals). During the hydrogenation of 3-nitrostyrene, the TOF numbers based on surface Pt atoms of Pt-1/Ni nanocrystals reached similar to 1800 h(-1) under 3 atm of H-2 at 40 degrees C, much higher than that of Pt single atoms supported on active carbon, TiO2 , SiO2 , and ZSM-S. Mechanistic studies reveal that the remarkable activity of Pt-1/Ni nanocrystals derived from sufficient hydrogen supply because of spontaneous dissociation of H-2 on both Pt and Ni atoms as well as facile diffusion of H atoms on Pt-1/Ni nanocrystals. Moreover, the ensemble composed of the Pt single atom and nearby Ni atoms in Pt-1/Ni nanocrystals leads to the adsorption configuration of 3-nitrostyrene favorable for the activation of nitro groups, accounting for the high selectivity for 3-vinylaniline.
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