含铁系元素的EU-1分子筛的水热晶化动力学  

Hydrothermal Crystallization Kinetics of EU-1 Zeolite Containing Iron Series of Elements

作　　者：杨冬花[1] 石宝宝[1] 王新波[1] 武正簧[1] 刘霞[1] 窦涛[2,3] 

机构地区：[1]太原理工大学化学化工学院,太原030024 [2]中国石油大学(北京)化学工程学院催化重点实验室,北京102249 [3]太原理工大学精细化工研究所,太原030024

出　　处：《高等学校化学学报》2013年第10期2363-2369,共7页Chemical Journal of Chinese Universities

基　　金：国家"九七三"计划项目(批准号:2012CB215002);国家自然科学基金(批准号:20973123);山西省自然科学基金(批准号:2013011041-1)资助

摘　　要：以实验室自制的溴化六甲双铵(HMBr2)为模板剂,通过水热法快速合成出含Fe,Co或Ni杂原子的EU-1分子筛.通过研究晶化过程中电位和相对结晶度的变化,得出了晶化过程中胶体粒子表面电荷及动力学参数.结果表明,Fe,Co或Ni的引入对EU-1分子筛晶核的形成有很好的促进作用,Fe,Co或Ni阳离子的空d轨道可以加速低聚物硅的形成,这些结构在晶化过程中加速了晶体的成核和生长,导致其成核时间明显缩短,成核速率和晶体生长速率显著加快,表观活化能减小.表观成核活化能E n大于表观生长活化能E g,说明成核过程是速率控制步骤,因此采用较高的晶化温度有利于含铁系元素的EU-1分子筛成核,且能加快晶体生长过程.The EU-I zeolites contained Fe, Co, Ni heteroatoms were quickly synthesized through the hydro- thermal crystallization procedure with laboratory self-made hexamethonium bromide （HMBr2 ） as a template. Studying the potential of crystallization process and relative crystallinity change in the crystallization process, we obtained colloid particle surface charge and kinetic parameters. The results show that metal Fe,Co, Ni introduced into the EU-1 zeolities had a very good role in promoting crystal nuclei formation. Iron, cobalt, nickel cations with empty d orbitals can accelerate the formation of oligomer silicon, the structures of which in the process of crystallization accelerated the nucleation and growth of crystals, leading to their nucleation time significantly to be shortened, the nucleation rate and crystal growth rate significantly to be speeded up, the ap- parent activation energy to be decreased. The apparent activation energy of nucleation En is greater than the apparent growth activation energy Es and the nucleation process is the rate controlling step. So the high crystal lization temperature is favourable for formating crystal nuclei of EU-1 zeolite which contained Fe, Co, Ni atoms and can accelerate the subsequent crystal growth process. Raising temperature needs to shorten the crys- tallization time appropriately, which is in order to prevent the emergence of other crystals. For zeolites synthe- sis, homogeneous and good dispersion gel-sol gel must be prepared at first, and the zeta potential is an impor tant index of the surface charge properties and stability. Thus the change of it is essential for the synthesis of zeolites.

关 键 词：EU-1分子筛 表观活化能 结晶动力学 ZETA电位 金属原子 

分 类 号：O643.1[理学—物理化学]