Abstract
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 study, we use the methanol coupling reaction on the SrTiO3(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 SrTiO3(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 SrTiO3(100) B termination can well explain the ambient-pressure XPS data of methanol on the single-crystal SrTiO3(100) surface at 250 °C. This work suggests that a choice of B termination of perovskites would be beneficial for the C-C coupling reaction of methanol.
| Original language | English |
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| Pages (from-to) | 7210-7216 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry C |
| Volume | 122 |
| Issue number | 13 |
| DOIs | |
| State | Published - Apr 5 2018 |
Funding
This research is sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. APXPS spectra were recorded at Beamline 23-ID-2 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704.