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，建立了变压吸附脱除低浓度NO的体系。在MFI分子筛上，单位质量吸附剂对NO的可逆吸附量随金属离子的变化大小顺序为：过渡金属离子、碱土金属离子、稀土金属离子、质子。NO在Cu-MFI或Ag-MFI分子筛上的可逆吸附量最大，而在Co-MFI沸石上的不可逆吸附量最大。随着MFI分子筛中铜或银离子含量的增加，NO在分子筛上的可逆量和不可逆量均呈正比增加。研究了硅铝比为5.6-50的各种沸石催化剂上2-甲基丙烯与氨的反应。高温下催化剂活性随B酸中心含量和…的平行变化H-MFI-40分子筛上H~+的Na~+取代和二异丙胺的预吸附对催化剂活性的影响较大，表现为B酸位上的胺化反应。催化剂活性与硅铝比的关系表明，2-甲基丙烯与氨反应的控制因素是疏水性、沸石结构和溴化酸性。最近在铜离子交换的ZSM-5沸石(Cu-ZSM-5)上发现了在氧气和二氧化硫存在下烃类选择性催化还原氮氧化物。即使在温度低至573K的氧化气氛中，反应也会继续进行。为了实现一氧化二氮的选择性还原，向反应料流中加入氧气是必要的。碳氢化合物浓度的增加增加了氮气的转化率，扩大了活性温度区域。结果表明，Cu-ZSM-5是一种较好的稀燃汽柴油发动机催化剂。较少

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