期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 18, 期 17, 页码 12093-12100出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cp00162a
关键词
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资金
- Ministry of Science and Technology (MOST)
- National Center for Theoretical Sciences (NCTS), Taiwan [MOST 103-2632-M-033-001-MY3, MOST 104-2113-M-033-010]
We elucidate the possibility of nitrogen-doped carbon nanotube as a robust catalyst for CO oxidation. We have performed first-principles calculations considering the spin-polarization effect to demonstrate the reaction of CO oxidation catalyzed by the nitrogen-doped carbon nanotube. The calculations show that O-2 species can be partially reduced with charge transfer from the nitrogen-doped carbon nanotube and directly chemisorbed on the C-N sites of the nitrogen-doped carbon nanotube. The partially reduced O-2 species at the C-N sites can further directly react with a CO molecule via the Eley-Rideal mechanism with the barriers of 0.45-0.58 eV for the different diameter of nanotube. Ab initio molecular dynamics (AIMD) simulations were performed and showed that the oxidation of CO occurs by the Eley-Rideal mechanism. The relationship between the curvature and reactivity of the nitrogen doped carbon nanotube was also unraveled. It appears that the barrier height of the rate-limiting step depends on the curvature of the nitrogen-doped carbon nanotube in the trend of (3,3)-NCNT < (4,4)-NCNT < (5,5)-NCNT (decreases with increased curvature). Using this relationship, we can predict the barriers for other N-doped carbon nanotubes with different tube diameters. Our results reveal that the nitrogen doped carbon nanomaterials can be a good, low-cost, and metal-free catalyst for CO oxidation.
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