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Mechanistic aspects of NH3-SCR reaction over CeO2/TiO2-ZrO2-SO42− catalyst: In situ DRIFTS investigation
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2017-10-04 , DOI: 10.1016/j.cej.2017.10.011
Jie Fan , Ping Ning , Zhongxian Song , Xin Liu , Lanying Wang , Jing Wang , Huimin Wang , Kaixian Long , Qiulin Zhang

The solid superacid TiO2-ZrO2-SO42−-supported 20 wt.% CeO2 catalyst (20CeO2/Ti-Zr-S) was synthesized for selective catalytic reduction of NO with NH3 (NH3-SCR). The NH3-SCR performance was significantly enhanced by the construction of strong acid sites on the surface of 20CeO2/Ti-Zr-S and over 96% NO conversion was obtained at 225–425 °C. Meanwhile, the strong interaction between solid superacid and CeO2 resulted in excellent redox property and abundant surface oxygen species. Furthermore, the NH3-SCR reaction over 20CeO2/Ti-Zr-S catalyst mainly followed the Langmuir-Hinshelwood mechanism at low-temperature (250 °C). The M-NO2 (M = Ce, Ti, Zr) nitrate compounds, monodentate and bridging nitrates were the crucial intermediates in Langmuir-Hinshelwood mechanism. In addition, amide (–NH2) species were available at 350 °C over 20CeO2/Ti-Zr-S catalyst, which facilitated the high-temperature NH3-SCR activity via Eley-Rideal pathway.



中文翻译:

CeO 2 / TiO 2 -ZrO 2 -SO 4 2-催化剂上NH 3 -SCR反应的机理:原位DRIFTS研究

合成了固体超强酸TiO 2 -ZrO 2 -SO 4 2-负载的20 wt。%CeO 2催化剂(20CeO 2 / Ti-Zr-S),用于用NH 3(NH 3 -SCR)选择性催化还原NO 。通过在20CeO 2 / Ti-Zr-S表面上形成强酸位,可以显着提高NH 3 -SCR性能,并且在225–425°C时获得超过96%的NO转化率。同时,固体超强酸与CeO 2之间的强相互作用导致优异的氧化还原性能和丰富的表面氧物种。此外,在20CeO 2上的NH 3 -SCR反应/ Ti-Zr-S催化剂在低温(250°C)下主要遵循Langmuir-Hinshelwood机理。M-NO 2(M = Ce,Ti,Zr)硝酸盐化合物,单齿硝酸盐和桥连硝酸盐是Langmuir-Hinshelwood机理的关键中间体。此外,在20CeO 2 / Ti-Zr-S催化剂上,可在350°C的温度下使用酰胺(–NH 2)物种,这有助于通过Eley-Rideal途径提高高温NH 3 -SCR的活性。

更新日期:2017-10-04
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