TY - JOUR
T1 - Understanding Methanol Coupling on SrTiO3 from First Principles
AU - Huang, Runhong
AU - Fung, Victor
AU - Zhang, Yafen
AU - Mullins, David R.
AU - Wu, Zili
AU - Jiang, De En
N1 - Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/4/5
Y1 - 2018/4/5
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85045054169&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcc.8b00273
DO - 10.1021/acs.jpcc.8b00273
M3 - Article
AN - SCOPUS:85045054169
SN - 1932-7447
VL - 122
SP - 7210
EP - 7216
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 13
ER -