中文摘要：

采用六亚甲基亚胺（HMI）为模板剂,合成了新型SAPO-35分子筛,研究发现SAPO-35的酸性随着硅铝摩尔比增加[n（SiO2）/n（Al2O3）=0.3,0.5,0.7]呈现先增加后降低的趋势,当n（Si）/n（Al）=0.7时,部分Si将发生SM3取代,进而降低SAPO-35酸量.进一步采用旋转浸渍法和离子交换法对SAPO-35进行改性,制得Cu/SAPO-35催化剂,并研究了其催化氨气选择性还原（NH3-SCR）反应的性能.催化剂表征结果表明,Cu主要以Cu^2＋离子形式存在于离子交换法制备的Cu/SAPO-35中,因此其NH3-SCR催化性能更优良.基于液相离子交换法,进一步研究了不同硅铝比[n（SiO2）/n（Al2O3）=0.3,0.5,0.7]SAPO-35原粉酸性对所制备Cu/SAPO-35催化剂NH3-SCR反应活性的影响,结果表明,分子筛原粉强酸量越大,制得的Cu基催化剂中Cu^2＋离子含量越高,从而催化剂的SCR活性、N2选择性更优.

英文摘要：

A new type of SAPO-35 zeolite was synthesized utilizing hexamethyleneimine（ HMI） as template.It was found that the acidity of SAPO-35 firstly increased and then decreased along with the increasing of SiO2/Al2O3 molar ratio（ 0. 3,0. 5,0. 7）. With the molar ratio of Si O2/ Al2O3= 0. 7,the SM3 substitution mode occurred for the atomic Si during the SAPO-35 synthesis process,which could decrease the related acidity.The impregnation and wet ion exchange（ WIE） method were applied to produce Cu modified SAPO-35 samples of Cu / SAPO-35, which were further evaluated in NH3-SCR reaction system. According to various characterization results of XRF,NH3-TPD,and H2-TPR,it was revealed that the cationic Cu^2＋constituted the main copper species on WIE method prepared Cu / SAPO-35,which displayed much better NH3-SCR catalytic performance with respect to that of Cu / SAPO-35 prepared by impregnation method. Finally,various Cu/SAPO-35 with different SiO2/ Al2O3 molar ratio（ 0. 3,0. 5,0. 7） were prepared by WIE and further evaluated for NH3-SCR,wherein the influences of the acidities of parent SAPO-35 were thereafter investigated. It was revealed that the higher acidity of parent SAPO-15 could produce higher amount of exchanged Cu^2＋cations,which resulted in superior NH3-SCR activity and N2 selectivity.