Optimization and Modeling of CuOx/OMWNT’s for Catalytic Reduction of Nitrogen Oxides by Response Surface Methodology

Mahnaz Pourkhalil
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引用次数: 1

Abstract

A series of copper oxide (CuOx) catalysts supported by oxidized multi-walled carbon nanotubes (OMWNT’s) were prepared by the wet impregnation method for the low temperature (200 °C) selective catalytic reduction of nitrogen oxides (NOx) using NH3 as a reductant agent in the presence of excess oxygen. These catalysts were characterized by FTIR, XRD, SEM-EDS, and H2-TPR methods. The response surface methodology was employed to model and optimize the effective parameters in the preparation of CuOx/OMWNT’s catalysts in NOx removal by NH3-SCR process. Three experimental parameters, including calcination temperature, calcination time, and CuOx loading were chosen as the independent variables. The central composite design was utilized to establish a quadratic model as a functional relationship between the conversion of NOx as a response factor and independent variables. The ANOVA results showed that the NOx conversion is significantly affected by calcination temperature and CuOx loading. At the optimal values of the studied parameters, the maximum conversion of NOx, 86.3 %, was obtained at a calcination temperature of 318 °C, a calcination time of 3.4 hr., and CuOx loading of 16.73 wt.%; the reaction conditions was as follows: T= 200 °C, P= 1 bar, NO = NH3 = 900 ppm, O2 = 5 vol.%, and GHSV = 30,000 hr.−1. The regression analysis with an R2value of 0.9908 revealed a satisfactory correlation between the experimental data and the values predicted for the conversion of NOx. The XRD and H2-TPR results of the best catalyst showed that the formation of CuO as the dominant phase of CuOx is the key factor in low temperature selective catalytic reduction (SCR) process.
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基于响应面法的CuOx/OMWNT催化还原氮氧化物的优化与建模
采用湿浸渍法制备了一系列氧化多壁碳纳米管(OMWNT’s)负载型氧化铜(CuOx)催化剂,在过量氧存在下,以NH3为还原剂,进行了低温(200℃)选择性催化还原氮氧化物(NOx)的研究。采用FTIR、XRD、SEM-EDS、H2-TPR等方法对催化剂进行了表征。采用响应面法对NH3-SCR法制备CuOx/OMWNT脱硝催化剂的有效参数进行了建模和优化。选取煅烧温度、煅烧时间、CuOx负载3个实验参数作为自变量。利用中心复合设计建立了作为响应因子的NOx转化率与自变量之间的函数关系的二次模型。方差分析结果表明,煅烧温度和CuOx负荷对NOx转化率有显著影响。在最佳参数下,当煅烧温度为318℃,煅烧时间为3.4 h时,NOx的最大转化率为86.3%。, CuOx负荷量为16.73 wt.%;反应条件为:T= 200℃,P= 1 bar, NO = NH3 = 900 ppm, O2 = 5 vol.%, GHSV = 30,000 hr。回归分析结果表明,实验数据与NOx转化率预测值具有较好的相关性,r2值为0.9908。最佳催化剂的XRD和H2-TPR结果表明,CuO作为CuOx的主导相的形成是低温选择性催化还原(SCR)过程的关键因素。
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