DESIGN AND DEVELOPMENT OF NOVEL CATALYTIC PROCESS UTILIZING ZEOLITE

1. 研究了不同金属交换沸石对NO的吸附性能，建立了变压吸附去除低浓度NO的体系。对于MFI沸石，每重量吸附剂对NO的可逆吸附量随金属离子的增加变化较大；过渡金属离子[j]；[)碱土金属离子>稀土金属离子[]y .apprxeq.[)质子。Cu-或Ag-MFI沸石对NO的可逆吸附量最大，而Co-MFI沸石对NO的不可逆吸附量最大。Cu-或Ag-MFI沸石对NO的可逆和不可逆吸附量与MFI沸石中Cu或Ag离子的量成正比增加。在硅铝比为5.6 ~ 50的沸石催化剂上，研究了2-甲基丙烯与氨的反应。H- mfi -40中Na^+取代H^+或二异丙胺的预吸附使活性显著降低，表明在Bronsted酸位点上发生了胺化反应。催化活性对二氧化硅/氧化铝比的依赖性表明，疏水性、沸石结构以及Brphinsted酸度是控制2-甲基丙烯与氨反应的因素。最近在铜离子交换的ZSM-5沸石（Cu- ZSM-5）上发现了在氧和二氧化硫存在下碳氢化合物选择性催化还原一氧化氮的现象。即使在温度低至573K的氧化气氛中，反应也能进行。在反应物流中加入氧气是实现一氧化氮选择性还原的必要条件。烃类浓度的增加增加了转化成氮的速度，扩大了反应的活跃温度范围。结果表明，Cu-ZSM-5是一种适用于稀燃汽油机和柴油机的催化剂。少

1. NO adsorption properties of various metal exchanged zeolites were studied to develop the system for removal of low concentration of NO by using pressure swing adsorption. With MFI zeolite, the amounts of reversible adsorption of NO per weight of adsorbent much changed with metal ion in the following order; transition metal ion(] SY.apprxeq.[)alkaline earth metal ion>rare earth metal ion(] SY.apprxeq.[)proton. The amounts of reversible adsorption of NO on Cu- or Ag-MFI zeolites were the largest while that of irreversible NO adsorption was the greatest on Co-MFI zeolite. The amount of reversible and irreversible adsorption of NO on Cu-or Ag-MFI zeolites increased in proportion to the amount of Cu or Ag ion in MFI zeolite.2. The reaction between 2-methylpropene and ammonia was investigated over various zeolite catalysts having a wide range of silica/alumina ratio of 5.6-50. A parallel change of the catalytic activity with the amount of Bronsted acid site at elevated temperatures and th … More e significant decrease of the activity by the Na^+ substitution of H^+ in H-MFI-40 or by the preadsorption of diisopropylamine showed the amination on Bronsted acid site.The dependence of the catalytic activity on silica/alumina ratio suggested that hydrophobicity and zeolite structure as well as Brphinsted acidity are factors controlling the reaction between 2-methylpropene and ammonia.3. Selective catalytic reduction of nitrogen monoxide by hydrocarbon in the presence of oxygen and sulphur dioxide has very recently been found on copper ion-exchanged ZSM-5 zeolite (Cu- ZSM-5). The reaction proceeds even in the oxidizing atmosphere at temperatures as low as 573K. Addition of oxygen to the reactant stream is necessary is achieve the selective reduction of nitrogen monoxide. The increment of concentration of hydrocarbon increased the conversion into nitrogen and expanded the active temperature region. It was concluded that Cu-ZSM-5 is suggested as one of the strong candidates for catalysts applicable to lean-burn gasoline and diesel engines. Less