王建,窦喆,潘燕飞,徐秀峰.MnxCo3-xO4复合氧化物及改性催化剂催化分解N2O[J].分子催化,2015,(3):246-255
MnxCo3-xO4复合氧化物及改性催化剂催化分解N2O
Catalytic Decomposition of N2O over MnxCo3-xO4 Mixed oxides and Modified Catalysts
投稿时间:2015-05-12  修订日期:2015-06-08
DOI:
中文关键词:  N2O催化分解, MnxCo3-xO4复合氧化物, 助剂钾前驱物, 钾负载量, 催化活性, 催化稳定性
英文关键词:Catalytic decomposition of N2O, MnxCo3-xO4 mixed oxides, additive potassium precursors, potassium loadings, catalytic activity, Catalytic stability
基金项目:山东省科技发展计划项目(2012GSF11708),烟台大学研究生科技创新基金项目(GIFYTU)
作者单位E-mail
王建 烟台大学 s0334139@163.com 
窦喆 烟台大学 xiufengxu68@sina.com 
潘燕飞 烟台大学 yfpan@ytu.edu.cn 
徐秀峰* 烟台大学 xxf@ytu.edu.cn 
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中文摘要:
      用共沉淀法制备了组成为Mn0.4Co2.6O4的尖晶石型复合氧化物,表面浸渍不同钾盐(K2CO3, KNO3, K2C2O4, CH3COOK)溶液制备K改性催化剂,用于催化分解N2O。用X射线衍射、N2物理吸附、红外光谱、扫描电镜、H2程序升温还原、X射线光电子能谱等技术表征了催化剂结构。考察了钾的前驱物和负载量对催化剂结构和活性的影响。结果表明:负载适量的K助剂弱化了催化剂表面Co-O和Mn-O键,使表面氧物种易脱除,提高了催化剂活性。优化出了活性较高的0.03K/Mn0.4Co2.6O4-500(K2CO3) 催化剂,制备参数是:以K2CO3溶液浸渍Mn0.4Co2.6O4复合氧化物,500C焙烧,K负载量为K/(Mn Co)=0.03(原子比)。有氧无水、有氧有水气氛400C连续反应50h,0.03K/Mn0.4Co2.6O4-500(K2CO3)催化剂上的N2O 转化率分别保持100%和74.2%,K改性催化剂稳定性较高。
英文摘要:
      Mn0.4Co2.6O4 spinel oxide was prepared by co-precipitation method, and incipiently impregnated by different potassium salts solution to prepare K-doped catalysts. These catalysts were applied in N2O decomposition reaction. The techniques such as X-ray diffraction (XRD), nitrogen physisorption, Fourier transformed infrared (FTIR), scanning electron microscopy (SEM), hydrogen temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) were used to characterize these catalysts. The effect of potassium precursors (K2CO3, KNO3, K2C2O4, and CH3COOK) and potassium loadings on catalytic activity was investigated. It is shown that the appropriate loading of potassium addition weakened the strength of Co-O and Mn-O bonds, promoted the removal of surface oxygen species, and improved the catalyst activity and stability. The most active catalyst for N2O decomposition was 0.03K/Mn0.4Co2.6O4-500(K2CO3) catalyst prepared by impregnating K2CO3 solution over Mn0.4Co2.6O4 with K/(Mn Co) atomic ratio of 0.03 and calcined at 500C, over which 100% and 74.2% conversion of N2O can be maintained at 400C after continuous running for 50h in oxygen alone and oxygen-steam together, respectively.
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