Investigation of the Poisoning Mechanism of Lead on the CeO2-WO3 Catalyst for the NH3-SCR Reaction via in Situ IR and Raman Spectroscopy Measurement

Investigation of the Poisoning Mechanism of Lead on the CeO2-WO3 Catalyst for the NH3-SCR Reaction via in Situ IR and Raman Spectroscopy Measurement
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通过原位红外和拉曼光谱测量研究铅对 NH3-SCR 反应 CeO2-WO3 催化剂的中毒机制

DOI:
10.1021/acs.est.6b02307
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发表时间:
2016-09-06
影响因子:
11.4
通讯作者:
Hao, Jiming
Hao, Jiming
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Peng, Yue;Si, Wenzhe;Hao, Jiming

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The in situ IR and Raman spectroscopy measurements were conducted to investigate lead poisoning on the CeO2-WO3 catalysts. The deactivation mechanisms were studied with respect to the changes of surface acidity, redox property, nitrate/nitrite adsorption behaviors, and key active sites (note that the results of structure activity relationship of CeO2-WO3 were based on our previous research). (1) Lewis acid sites originated from CeO2 and crystalline WO3, whereas Bronsted acid sites originated from Ce-2(WO4)(3). The poisoned catalysts exhibited a lower surface acidity than the fresh catalysts: the number of acid sites decreased, and their thermal stability weakened. (2) The reducibility of catalysts and the amount of active oxygen exhibited a smaller influence after poisoning because lead preferred to bond with surface WOx species rather than CeO2. (3) The quantity of active nitrate species decreased due to the lead coverage on the catalyst and the partial bridged-nitrate species induced by lead exhibited a low degree of activity at 200 degrees C. (4) Crystalline WO3 and Ce-2(WO4)(3) originated from the transformation of polytungstate sites. These sites were the key active sites during the SCR process. The formation temperatures of polytungstate on the poisoned catalysts were higher than those on the fresh catalysts.