杨冬花,石宝宝,代蓉,郭超,王新波,窦涛,武正簧,韩培德.ITQ-13分子筛合成及酸性的DFT理论计算研究[J].分子催化,2014,(6):564-573
ITQ-13分子筛合成及酸性的DFT理论计算研究
Synthesis and Density Functional Theory Studies on the Acidity of ITQ - 13 Molecular Sieve
投稿时间:2014-09-16  修订日期:2014-10-30
DOI:
中文关键词:  ITQ-13分子筛  合成  Ge、B、Al同晶取代  DFT理论
英文关键词:ITQ-13molecular sieve  synthesis  Ge, B, Al isomorphous substitution  density functional theory
基金项目:国家重点基础研究发展计划(973计划);国家自然科学基金项目(面上项目,重点项目,重大项目)
作者单位E-mail
杨冬花* 太原理工大学 ydh1962@163.com 
石宝宝 太原理工大学 437920223@qq.com 
代蓉 太原理工大学 845489063@qq.com 
郭超 中国矿业大学力建学院(北京) 772308829@qq.com 
王新波 太原理工大学 517004103@qq.com 
窦涛 太原理工大学 dtaol@163.com 
武正簧 太原理工大学 wzh-li@163.com 
韩培德 太原理工大学 hanpeide@126.com 
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中文摘要:
      本论文以氢氧化已烷双铵(R(OH)2)和溴化六甲双铵(HMBr2)为模板剂分别合成了ITQ-13、B-ITQ-13、Al-ITQ-13分子筛,采用XRD、SEM-EDX、N2吸附-脱附、FT-IR、MAS NMR等手段对合成的分子筛进行表征,比较了两种模板剂合成的ITQ-13分子筛的性质,以溴化六甲双铵(HMBr2)为模板剂,在碱性加晶种的条件下,反应3~10天合成出了ITQ-13以及含杂原子B、Al的ITQ-13分子筛,降低了合成的成本。以溴化六甲双铵为模板剂合成的ITQ-13晶貌有块状和球形针状堆积混合晶貌组成,孔道宽,晶粒因堆积形成的介孔居多。量子力学中的密度泛函理论(DFT)计算Ge、B、Al同晶取代Si在ITQ-13分子筛9个不同T位的分布,T5位对于ITQ-13分子筛的特殊骨架结构形成具有重要作用,对于骨架的电荷平衡以及几何约束力都有重要作用。Al原子容易替代的位置是位于九元环和十元环孔口相交处的T6、T7位。
英文摘要:
      ITQ-13、B-ITQ-13、Al-ITQ-13 zeolites were synthesized by using hydroxide hexane dual ammonium (R(OH)2) and hexamethonium bromide as templates. The properties of prepared ITQ-13 zeolites which synthesized with two templates were compared, and characterized by XRD, SEM-EDX, N2 adsorption-desorption, FT-IR, and MAS NMR. Under the condition of alkaline with seed, and over 3~10 days, ITQ-13, B-ITQ-13, Al-ITQ-13 were synthesized when the template was hexamethonium bromide, bringing down the cost of synthesis. The morphology of ITQ-13 zeolites which was synthesized through this method presents block and spherical acicular accumulation of mixed crystal appearance .The sample accumulation form the mesoporous majority and has wide channel. The substitution of framework Ge、B、Al at 9 T sites of ITQ-13 zeolite was calculated by using the method of density functional theory. T5 site plays an important role in the formation of the special sieve structure of ITQ-13 molecular; it also has an important function in the skeleton of charge balance and geometric binding. The sites that A1 can easily replace were located at sites of T6、T7 where 9-ring and 10-ring cross.
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