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This content will become publicly available on March 19, 2019

Title: Understanding Methanol Coupling on SrTiO 3 from First Principles

Perovskites are interesting materials for catalysis due to their great tunability. However, the correlation of many reaction processes to the termination of a perovskite surface is still unclear. In this paper, we use the methanol coupling reaction on the SrTiO 3(100) surface as a probe reaction to investigate direct C–C coupling from a computational perspective. We use density functional theory to assess methanol adsorption, C–H activation, and direct C–C coupling reactions on the SrTiO 3(100) surface of different terminations. We find that, although methanol molecules dissociatively adsorb on both A and B terminations with similar strength, the dehydrogenation and C–C coupling reactions have significantly lower activation energies on the B termination than on the A termination. The predicted formation of methoxy and acetate on the SrTiO 3(100) B termination can well explain the ambient-pressure XPS data of methanol on the single-crystal SrTiO 3(100) surface at 250 °C. Finally, this work suggests that a choice of B termination of perovskites would be beneficial for the C–C coupling reaction of methanol.
Authors:
 [1] ; ORCiD logo [1] ;  [2] ; ORCiD logo [2] ; ORCiD logo [3] ; ORCiD logo [1]
  1. Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division. Center for Nanophase Materials Sciences
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231; SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 13; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of California, Riverside, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1435220