Synthesis and kinetics investigation of meso-microporous Cu-SAPO-34 catalysts for the selective catalytic reduction of NO with ammonia

Synthesis and kinetics investigation of meso-microporous Cu-SAPO-34 catalysts for the selective catalytic reduction of NO with ammonia
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DOI:
10.1016/j.jes.2016.01.027
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发表时间:
2016-10-01
影响因子:
6.9
通讯作者:
Sun, Qianyao
Sun, Qianyao
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Liu, Jixing;Yu, Fuhong;Sun, Qianyao

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采用一锅水热晶化法制备了一系列介孔微孔CuSAPO-34催化剂,这些催化剂在低温下表现出优异的NH3-SCR性能。采用X射线衍射仪、扫描电子显微镜、透射电子显微镜、氮气吸附-脱附、核磁共振、电感耦合等离子体原子发射光谱仪、X射线吸收光谱仪、氨程序升温脱附、紫外可见漫反射光谱、程序升温还原等手段对其结构和物化性能进行了表征。分析结果表明,Cu-SAPO-34催化剂的高活性可以归因于氧化还原性能的增强、中孔的形成和更多的酸性中心。此外,动力学结果还证明,介孔的形成显著降低了扩散阻力,从而提高了反应物对催化活性中心的可及性。在150-425℃的宽活性温度范围内,1.0-Cu-SAPO-34催化剂表现出较高的NO转化率(>90%)。爱思唯尔出版公司(Elsevier B.V.)
A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH3-SCR performance at low temperature. Their structure and physic chemical properties were characterized by means of X-ray diffraction patterns (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), N-2 sorption-desorption, nuclear magnetic resonance (NMR), Inductively Coupled Plasma-Atomic Emission spectrometer (ICP-AES), X-ray absorption spectroscopy (XPS), Temperature-programmed desorption of ammonia (NH3-TPD), Ultraviolet visible diffuse reflectance spectroscopy (UV-Vis DRS) and Temperature programmed reduction (TPR). The analysis results indicate that the high activities of Cu-SAPO-34 catalysts could be attributed to the enhancement of redox property, the formation of mesopores and the more acid sites. Furthermore, the kinetic results verify that the formation of mesopores remarkably reduces diffusion resistance and then improves the accessibility of reactants to catalytically active sites. The 1.0-Cu-SAPO-34 catalyst exhibited the high NO conversion (>90%) among the wide activity temperature window in the range of 150-425 degrees C. (C) 2016 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.