Mechanism of the selective catalytic reduction of NOx by C2H5OH over Ag/Al2O3

Mechanism of the selective catalytic reduction of NOx by C2H5OH over Ag/Al2O3
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DOI:
10.1016/j.apcatb.2003.12.004
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发表时间:
2004-05
影响因子:
22.1
通讯作者:
Yunbo Yu;Hong He;Qingcai Feng;Hongwei Gao;Xin Yang
Yunbo Yu;Hong He;Qingcai Feng;Hongwei Gao;Xin Yang
中科院分区:
化学1区
文献类型:
--
作者:
Yunbo Yu;Hong He;Qingcai Feng;Hongwei Gao;Xin Yang

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The mechanism of the selective catalytic reduction (SCR) of NOxby C2H5OH over silver catalyst (Ag/Al2O3) was investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Attention was focused on the formation and reactivity of novel enolic species on the Ag/Al2O3surface. DRIFTS spectra show that the surface enolic species, which was derived from partial oxidation of C2H5OH over Ag/Al2O3in the presence of excess oxygen, play a crucial role in the formation of isocynate species (NCO) by reaction with NO+O2or NO3−absorbed on the surface of Ag/Al2O3. 2,3-dihydrofuran was used to an enolic model compound in our DRITFS study, and the results support our assignment. A novel mechanism of the SCR of NOxby C2H5OH is proposed based on the DRIFTS studies. The mechanistic differences between the SCR of NOxby C2H5OH and that by C3H6are discussed. The high reactivity of the enolic species results in high surface concentration of NCO and high efficiency of NOxreduction using C2H5OH as a reductant. The results of density functional theory (DFT) calculations are in good agreement with the DRIFTS spectra, and support our suggestions about the surface enolic species.