| Title: |
Low-Temperature Propylene Epoxidation Activity of CuO–CeO2Catalyst with CO + O2: Role of Metal–Support Interaction on the Reducibility and Catalytic Property of CuOxSpecies |
| Authors: |
Baidya, Tinku, Mazumder, Tanmoy, Koltunov, Konstantin Yu., Likhar, Pravin R., Clark, Adam H., Tiwari, Khushubo, Sobolev, Vladimir I., Payra, Soumitra, Murayama, Toru, Lin, Mingyue, Bera, Parthasarathi, Roy, Sounak, Biswas, Krishanu, Safonova, Olga, Srinivasa Rao, Bolla, Haruta, Masatake |
| Source: |
The Journal of Physical Chemistry - Part C; July 2020, Vol. 124 Issue: 26 p14131-14146, 16p |
| Abstract: |
Epoxidation of propylene into propylene oxide (PO) in the gas phase is a highly challenging reaction. Cu-based catalysts have been active for this reaction, but the state of Cu as an active species is still debatable. In this paper, we report the propylene epoxidation activity of solution combustion synthesized Cu/CeO2catalysts with the CO + O2mixture at low temperatures (50–100 °C) peaking at ∼80 °C. The highest PO yield was obtained with 20–25% Cu loading in CeO2. In contrast, the reaction over the catalyst containing nonreducible support such as Cu/SiO2occurred above 170 °C. Detailed structural characterization indicated two types of Cu species such as Cu2+partly (∼3%) dissolved in CeO2forming a CuxCe1–xO2−δphase and the remaining amount formed highly dispersed CuO as a separate phase. Thus, the highest activity relates to the optimum presence of CuO along with Ce1–xCuxO2−δ. The reducibility of the Cu species in two phases was significantly shifted toward lower temperatures, indicating strong electronic interaction between the two phases. The substituted Cu2+was reduced first, and then, the bulk CuO reduction was initiated. In situ spectroscopic studies showed Cu+formation from Cu2+over Cu/CeO2catalysts even at room temperature unlike in CeO2or CuO + CeO2physical mixtures, indicating strong electronic interaction between Ce1–xCuxO2−δand CuO phases on CO adsorption in the Cu/CeO2catalyst. It is proposed that substituted Cu2+along with Ce4+is reduced easily, and then, Ce3+promotes the reduction of the interfacial CuO phase that might donate active oxygen species for epoxidation reaction. |
| Database: |
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