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H3PW12O40在NH3选择性催化还原NO中促进作用机制的漫反射傅里叶变换红外光谱(DRIFT)研究

DRIFT studies on promotion mechanism of H3PW12O40 in selective catalytic reduction of NO with NH3.

作者信息

Weng Xiaole, Dai Xiaoxia, Zeng Qingshan, Liu Yue, Wu Zhongbiao

机构信息

Department of Environmental Engineering, Zhejiang University, Yuhangtang Road 388, Hangzhou 310058, China.

Department of Environmental Engineering, Zhejiang University, Yuhangtang Road 388, Hangzhou 310058, China; Zhejiang Provincial Engineering Research Center of Industrial Boiler & Furnace Flue Gas Pollution Control, Yuhangtang Road 388, Hangzhou 310058, China.

出版信息

J Colloid Interface Sci. 2016 Jan 1;461:9-14. doi: 10.1016/j.jcis.2015.09.004. Epub 2015 Sep 5.

Abstract

Heteropoly acids (HPAs) have been effectively utilized in selective catalytic reduction (SCR) of NO to improve the NH3 absorption capacity and alkaline/alkali metal resistance for SCR catalysts. However, despite the promise on super-acidities, their other properties that would work on SCR process are still lack of exploration. In this study, a 12-tungstaphosphoric acid (H3PW12O40, HPW) was selected to modify a well-reported CeO2 catalyst. The resulted CeO2/HPW catalyst was subsequently utilized for SCR of NO with excess NH3, which revealed a significantly promoted performance in SCR reaction. DRIFT analyses showed that the unique NO2 absorption capacity of HPW could prevent the NO2 being further oxidized into nitrate species and the abundant Brønsted acid sites could effectively retain the NH3, avoiding them being over-oxidized at evaluated temperatures. The presence of NO2 was demonstrated able to induce a so called "fast SCR" reaction over the CeO2/HPW catalyst, which effectively facilitated the SCR reaction. Furthermore, we have also constructed a CeO2@HPW catalyst, which showed an enhanced SO2 poisoning resistance in SCR reaction.

摘要

杂多酸(HPAs)已被有效地用于将NO选择性催化还原(SCR),以提高SCR催化剂的NH₃吸收能力和耐碱性/碱金属性。然而,尽管杂多酸具有超强酸性的前景,但它们在SCR过程中起作用的其他性质仍缺乏探索。在本研究中,选择了12-钨磷酸(H₃PW₁₂O₄₀,HPW)来改性一种广为人知的CeO₂催化剂。随后将所得的CeO₂/HPW催化剂用于过量NH₃存在下的NO的SCR反应,结果表明该催化剂在SCR反应中表现出显著提高的性能。漫反射红外傅里叶变换光谱(DRIFT)分析表明,HPW独特的NO₂吸收能力可防止NO₂进一步氧化成硝酸盐物种,且丰富的布朗斯特酸位点可有效保留NH₃,避免其在评估温度下被过度氧化。结果表明,NO₂的存在能够在CeO₂/HPW催化剂上引发所谓的“快速SCR”反应,从而有效促进SCR反应。此外,我们还构建了一种CeO₂@HPW催化剂,该催化剂在SCR反应中表现出增强的抗SO₂中毒能力。

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