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介孔-微孔 Cu-SAPO-34 催化剂的合成及其用于氨选择性催化还原 NO 的动力学研究。

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

机构信息

State Key Laboratory of Heavy Oil Processing and Beijing Key Lab of Oil & Gas Pollution Control, China University of Petroleum, Changping, Beijing 102249, P. R. China.

Shandong Hengsheng Chemical Co., Ltd., Shandong 253024, China.

出版信息

J Environ Sci (China). 2016 Oct;48:45-58. doi: 10.1016/j.jes.2016.01.027. Epub 2016 Apr 30.

Abstract

A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH-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 sorption-desorption, nuclear magnetic resonance (NMR), Inductively Coupled Plasma-Atomic Emission spectrometer (ICP-AES), X-ray absorption spectroscopy (XPS), Temperature-programmed desorption of ammonia (NH-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°C.

摘要

一系列中孔-微孔 Cu-SAPO-34 催化剂通过一锅水热结晶法成功合成,这些催化剂在低温下表现出优异的 NH-SCR 性能。通过 X 射线衍射图谱 (XRD)、扫描电子显微镜 (SEM)、透射电子显微镜 (TEM)、N 吸附-解吸、核磁共振 (NMR)、电感耦合等离子体-原子发射光谱仪 (ICP-AES)、X 射线吸收光谱 (XPS)、氨程序升温脱附 (NH-TPD)、紫外可见漫反射光谱 (UV-Vis DRS) 和程序升温还原 (TPR) 对其结构和物理化学性质进行了表征。分析结果表明,Cu-SAPO-34 催化剂的高活性可归因于氧化还原性能的增强、中孔的形成和更多的酸性位。此外,动力学结果证实了中孔的形成显著降低了扩散阻力,从而提高了反应物进入催化活性位的可及性。在 150-425°C 的宽活性温度窗口范围内,1.0-Cu-SAPO-34 催化剂表现出高的 NO 转化率 (>90%)。

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