Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 121, Issue 9, Pages 4970-4979Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b11175
Keywords
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Funding
- National Natural Science Foundation of China [U1462110]
- National Natural Science Foundation of China (NSFC) Research Fund for International Young Scientists FY [21650110450]
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Anatase TiO2 nanosheets (TiO2-NS) and nanospindles (TiO2-NSP) have been successfully prepared with F-and glacial acetic acid as structure -directing agents, respectively. The Fe2O3/TiO2-NS and Fe2O3/TiO2-NSP nanocatalysts were prepared by a wet incipient impregnation method with a monolayer amount of Fe2O3. All the catalysts were employed for the selective catalytic reduction of NO with NH3 (NH3-SCR) in order to understand the morphology dependent effects. It is interesting that the Fe2O3/TiO2-NS nanocatalyst exhibited better removal efficiency of NOx in the temperature range of 100-450 degrees C, which was attributed to more oxygen defects and active oxygen, acid sites, as well as adsorbed nitrate species based on Raman spectra, XPS, NH3-TPD, NO+O-2-TPD, and in situ DRIFTS. The density functional theory (DFT) method was used to clarify the NO and NH3 adsorption abilities over the catalyst models of Fe2O3/TiO2{001} and Fe2O3/TiO2{101}. The results showed that the NH3 adsorption energy over the TiO2{001} (-2.00 eV) was lower than that over TiO2{101} (-1.21 eV), and the NO adsorption energy over TiO2{001} (-1.62 eV) was also lower than that over TiO2{101} (-0.29 eV), which agreed well with the experimental results that Fe2O3/TiO2-NS achieved higher catalytic activity than Fe2O3/TiO2-NSP for NH3-SCR of NO. In addition, the rapid electron transfer and regeneration of Fe3+ on the {001} facet of Fe2O3/TiO2-NS also promoted the NH3-SCR reaction efficiency. This work paves a way for understanding the facet-activity relationship of Fe2O3/TiO2 nanocatalysts in the NH3-SCR reaction.
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