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Title: Oxygen-Promoted Methane Activation on Copper

The role of oxygen in the activation of C–H bonds in methane on clean and oxygen-precovered Cu(111) and Cu 2O(111) surfaces was studied with combined in situ near-ambient-pressure scanning tunneling microscopy and X-ray photoelectron spectroscopy. Activation of methane at 300 K and “moderate pressures” was only observed on oxygen-precovered Cu(111) surfaces. Density functional theory calculations reveal that the lowest activation energy barrier of C–H on Cu(111) in the presence of chemisorbed oxygen is related to a two-active-site, four-centered mechanism, which stabilizes the required transition-state intermediate by dipole–dipole attraction of O–H and Cu–CH 3 species. Furthermore, the C–H bond activation barriers on Cu 2O(111) surfaces are large due to the weak stabilization of H and CH 3 fragments.
Authors:
 [1] ;  [2] ;  [3] ; ORCiD logo [3] ;  [4] ;  [5] ; ORCiD logo [5] ; ORCiD logo [5]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Nanjing Univ. of Science & Technology, Xiaolingwei (China)
  2. Xi'an Jiaotong Univ., Xi'an (China)
  3. State Univ. of New York, Binghamton, NY (United States)
  4. Harvard Univ., Cambridge, MA (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-114713-2017-JA
Journal ID: ISSN 1520-6106; KC0403020; TRN: US1800182
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 122; Journal Issue: 2; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY
OSTI Identifier:
1411144