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Reaction behaviors of CH3CN catalytic combustion over CuCeOx-HZSM-5 composite catalysts: The mechanism of enhanced N2 selectivity
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2019-12-06 , DOI: 10.1016/j.apcata.2019.117373
Yuxing Wang , Qingji Ying , Yaoyu Zhang , Yue Liu , Zhongbiao Wu

In this paper, the reaction behaviors of CH3CN catalytic combustion over CuCeOx-HZSM-5 catalysts prepared by the physical mixing and wet impregnation methods were investigated. The experimental results had revealed that the composite catalysts exhibited excellent degradation efficiency and high N2 selectivity: the Cu-Ce oxides ensured the high activity, and the introduction of HZSM-5 limited the formation of NOx. The involved reaction mechanism was then studied by an in situ DRIFT analysis. It could be deduced that different reaction pathways would occur over CuCeOx and HZSM-5. The catalytic reaction over CuCeOx mainly proceeded via an oxidation pathway. The CN group could be converted to isocyanate species [NCO(a)] which would be further oxidized to NOx. Over HZSM-5, CH3CN was mainly hydrolyzed into ammonia. For the CuCeOx-HZSM-5 composite catalysts, the over-oxidation of NCO(a) and NH3 was inhibited, and an internal selective catalytic reduction (SCR) reaction could occur, thereby greatly improving the N2 selectivity.



中文翻译:

CH 3 CN在CuCeO x -HZSM-5复合催化剂上的催化燃烧反应行为:N 2选择性增强的机理

研究了物理混合和湿法浸渍法制备的CuCeO x -HZSM-5催化剂上CH 3 CN催化燃烧的反应行为。实验结果已经表明,该复合催化剂表现出优异的降解效率和高氮2选择性:所述Cu-的Ce氧化物确保了高的活性,并引入HZSM-5的限制NO的形成X。然后通过原位DRIFT分析研究了所涉及的反应机理。可以推断出在CuCeO x和HZSM-5上会发生不同的反应途径。CuCeO x上的催化反应主要通过氧化途径进行。CN基团可以转化为异氰酸酯类[NCO(a)],后者会进一步氧化成NO x。在HZSM-5上,CH 3 CN主要水解成氨。对于CuCeO x -HZSM-5复合催化剂,可以抑制NCO(a)和NH 3的过度氧化,并且可以发生内部选择性催化还原(SCR)反应,从而大大提高了N 2的选择性。

更新日期:2019-12-07
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