A density functional theory study of propylene epoxidation on RuO2(110) surface

Atmaca D. O., Duzenli D., Ozbek M. O., ÖNAL I.

APPLIED SURFACE SCIENCE, cilt.385, ss.99-105, 2016 (SCI-Expanded) identifier identifier

  • Yayın Türü: Makale / Tam Makale
  • Cilt numarası: 385
  • Basım Tarihi: 2016
  • Doi Numarası: 10.1016/j.apsusc.2016.05.090
  • Dergi Adı: APPLIED SURFACE SCIENCE
  • Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus
  • Sayfa Sayıları: ss.99-105
  • Anahtar Kelimeler: DFT, RuO2, Propylene epoxidationa, TOTAL-ENERGY CALCULATIONS, PARTIAL OXIDATION, MOLECULAR-OXYGEN, COPPER, OXIDE, REACTIVITY, MECHANISM, CATALYSTS, ETHYLENE, ATOMS
  • Orta Doğu Teknik Üniversitesi Adresli: Evet

Özet

Propylene epoxidation is investigated on RuO2(110) and oxygen added RuO2-O-ot(110) surfaces by periodic DFT computational method. The desired product propylene oxide (PO) as well as the undesired products acetone (AC) or propionaldehyde (PA) form on both surfaces through either surface intermediate oxometallopropylene (OMMP) or direct oxygen insertion mechanisms. On RuO2(110) surface, nucleophilic lattice oxygen at bridge position (O-br) favors the stable surface intermediate mechanism where high energy requirements for forward reactions are demonstrated in our calculations. On RuO2-O-ot(110) surface, however, higher reactivity of the electrophilic oxygen (Oot) species lowers the reaction barriers and enables an exothermic reaction path to the direct oxygen insertion for PO production. Therefore, RuO2-Oot surface is expected to show a higher PO rate. (C) 2016 Published by Elsevier B.V.