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一锅水热合成铜铋共掺杂介孔β沸石用于通过氨选择性催化还原去除氮氧化物

One-pot hydrothermal synthesis of CuBi co-doped mesoporous zeolite Beta for the removal of NOx by selective catalytic reduction with ammonia.

作者信息

Xie Zhiguo, Zhou Xiaoxia, Wu Huixia, Chen Lisong, Zhao Han, Liu Yan, Pan Linyu, Chen Hangrong

机构信息

State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Changning District, Shanghai 200050, P.R. China.

The Key Laboratory of Resource Chemistry of Ministry of Education and the Shanghai Key Laboratory of the Rare Earth Functional Materials. Shanghai Normal University, 100 Guilin Road, Xuhui District, Shanghai 200234, P.R. China.

出版信息

Sci Rep. 2016 Jul 22;6:30132. doi: 10.1038/srep30132.

Abstract

A series of CuBi co-doped mesoporous zeolite Beta (CuxBiy-mBeta) were prepared by a facile one-pot hydrothermal treatment approach and were characterized by XRD, N2 adsorption-desorption, TEM/SEM, XPS, H2-TPR, NH3-TPD and in situ DRIFTS. The catalysts CuxBiy-mBeta were applied to the removal of NOx by selective catalytic reduction with ammonia (NH3-SCR), especially the optimized Cu1Bi1-mBeta achieved the high efficiency for the removal of NOx and N2 selectivity, superior water and sulfur resistance as well as good durability. The excellent catalytic performance could be attributed to the acid sites of the support and the synergistic effect between copper and bismuth species. Moreover, in situ DRIFTS results showed that amides NH2 and NH4(+) generated from NH3 adsorption could be responsible for the high selective catalytic reduction of NOx to N2. In addition, a possible catalytic reaction mechanism on Cu1Bi1-mBeta for the removal of NOx by NH3-SCR was proposed for explaining this catalytic process.

摘要

通过简便的一锅水热法制备了一系列铜铋共掺杂的介孔β沸石(CuxBiy-mBeta),并采用XRD、N2吸附-脱附、TEM/SEM、XPS、H2-TPR、NH3-TPD和原位DRIFTS对其进行了表征。将催化剂CuxBiy-mBeta应用于氨选择性催化还原(NH3-SCR)去除NOx,特别是优化后的Cu1Bi1-mBeta在去除NOx和N2选择性方面表现出高效率,具有优异的耐水和耐硫性能以及良好的耐久性。优异的催化性能可归因于载体的酸性位点以及铜和铋物种之间的协同效应。此外,原位DRIFTS结果表明,NH3吸附产生的酰胺NH2和NH4(+)可能是NOx高选择性催化还原为N2的原因。此外,还提出了Cu1Bi1-mBeta上通过NH3-SCR去除NOx的可能催化反应机理来解释这一催化过程。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9eb/4957122/cf84c800016f/srep30132-f1.jpg

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