室温消除NO催化剂的研究
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摘要
本论文研究铜锰复合氧化物和活性炭负载金属氧化物催化剂,主要考察了在不引入还原剂的情况下,催化剂的室温消除NO的催化性能,以实现空气污染物的净化目的。
论文采用两次沉淀法制备了铜锰复合氧化物催化剂,深入地研究了各种制备参数对催化剂室温消除NO催化活性的影响,这些参数包括原料液[Cu]／[Mn]比、焙烧温度和焙烧时间,进而确定了催化剂的最佳制备条件,制备的催化剂具有较好的活性和稳定性,且具有很好的再生能力。用XRD、XPS技术对催化剂进行表征,研究了不同焙烧温度下的催化剂的微观结构和物相组成,并与催化剂活性相关联；用FTIR技术在线持续观察反应过程中催化剂表面的吸附变化,探究了反应机理。并将该催化剂与商业化的霍加拉特剂催化剂、二氧化锰和碳酸铜进行比较,考察不同催化剂的活性差异,结果表明该催化剂并非单纯的铜锰氧化物组成,而是形成了复杂的络合物。采用等体积浸渍法制备了Cr03／AC等一系列活性炭负载金属氧化物催化剂,并考察了这些催化剂对NO的催化活性。此外,采用掺杂金属氧化物和等离子体处理手段对铜锰复合氧化物催化剂进行了活性改性研究,虽然没有得到更好催化活性的催化剂,但是从中总结了一些经验。
在不引入还原剂的情况下,铜锰复合氧化物和活性炭负载金属氧化物催化剂都具有良好室温消除NO的催化活性,可用作空气净化催化材料。
In this thesis, copper-manganese oxide catalysts and metal oxide supported activated carbon catalysts were studied. Without the introduction of reducing agent, the purpose of purification of air pollutants was achieved. Catalytic properties of these catalysts for NO elimination at room temperature were mainly investigated.
A series of copper manganese oxide catalysts were prepared using re-precipitation procedure, in particular, the effect of arrange of preparation variables were investigated in detail. The variables investigated include [Cu]/ [Mn] ratio, calcination temperatures and calcination times. The optimum prepatation conditions were identified with respect to the catalyst activity for NO elimination at room temperature. The results showed that copper manganese oxide catalysts exhibited high catalytic activity, long-term stability, and good regeneration. The catalysts calcined at different temperatures were characterized by XRD and XPS techniques. The microstructure and phase were obtained and related to the catalytic activity reasonably. The reaction mechanism was investigated by in-situ FTIR. The different catalytic performances of commercial hopcalite, manganese dioxide, copper carbonate and copper manganese oxide for NO elimination were studied. However, copper manganese oxides were found to be in the formation of complicated complex but not a mix. A series of metal oxide supported actived carbon catalysts were prepared by impregnation procedure, and the catalytic activity on NO emilination was studied. In addition, catalytic performances of copper manganese oxide modied with doped metal oxides and pretreatment by plasma were studied. Although no better catalytic activity was found, some valuable experiences were obtained.
In summarize, without the introduction of reducing agent, copper manganese oxides and metal oxide supported activated carbon catalysts exhibited high catalytic activity for NO elimination at room temperature, which can be applied to air purification in the future.
论文采用两次沉淀法制备了铜锰复合氧化物催化剂,深入地研究了各种制备参数对催化剂室温消除NO催化活性的影响,这些参数包括原料液[Cu]／[Mn]比、焙烧温度和焙烧时间,进而确定了催化剂的最佳制备条件,制备的催化剂具有较好的活性和稳定性,且具有很好的再生能力。用XRD、XPS技术对催化剂进行表征,研究了不同焙烧温度下的催化剂的微观结构和物相组成,并与催化剂活性相关联；用FTIR技术在线持续观察反应过程中催化剂表面的吸附变化,探究了反应机理。并将该催化剂与商业化的霍加拉特剂催化剂、二氧化锰和碳酸铜进行比较,考察不同催化剂的活性差异,结果表明该催化剂并非单纯的铜锰氧化物组成,而是形成了复杂的络合物。采用等体积浸渍法制备了Cr03／AC等一系列活性炭负载金属氧化物催化剂,并考察了这些催化剂对NO的催化活性。此外,采用掺杂金属氧化物和等离子体处理手段对铜锰复合氧化物催化剂进行了活性改性研究,虽然没有得到更好催化活性的催化剂,但是从中总结了一些经验。
在不引入还原剂的情况下,铜锰复合氧化物和活性炭负载金属氧化物催化剂都具有良好室温消除NO的催化活性,可用作空气净化催化材料。
In this thesis, copper-manganese oxide catalysts and metal oxide supported activated carbon catalysts were studied. Without the introduction of reducing agent, the purpose of purification of air pollutants was achieved. Catalytic properties of these catalysts for NO elimination at room temperature were mainly investigated.
A series of copper manganese oxide catalysts were prepared using re-precipitation procedure, in particular, the effect of arrange of preparation variables were investigated in detail. The variables investigated include [Cu]/ [Mn] ratio, calcination temperatures and calcination times. The optimum prepatation conditions were identified with respect to the catalyst activity for NO elimination at room temperature. The results showed that copper manganese oxide catalysts exhibited high catalytic activity, long-term stability, and good regeneration. The catalysts calcined at different temperatures were characterized by XRD and XPS techniques. The microstructure and phase were obtained and related to the catalytic activity reasonably. The reaction mechanism was investigated by in-situ FTIR. The different catalytic performances of commercial hopcalite, manganese dioxide, copper carbonate and copper manganese oxide for NO elimination were studied. However, copper manganese oxides were found to be in the formation of complicated complex but not a mix. A series of metal oxide supported actived carbon catalysts were prepared by impregnation procedure, and the catalytic activity on NO emilination was studied. In addition, catalytic performances of copper manganese oxide modied with doped metal oxides and pretreatment by plasma were studied. Although no better catalytic activity was found, some valuable experiences were obtained.
In summarize, without the introduction of reducing agent, copper manganese oxides and metal oxide supported activated carbon catalysts exhibited high catalytic activity for NO elimination at room temperature, which can be applied to air purification in the future.
引文
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