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二丙胺的结构微调对磷酸铝分子筛晶化过程影响的凝胶组成依赖性
  • ISSN号:1001-4861
  • 期刊名称:《无机化学学报》
  • 时间:0
  • 分类:O611.4[理学—无机化学;理学—化学] O613.62[理学—无机化学;理学—化学]
  • 作者机构:吉林大学无机合成与制备化学国家重点实验室,吉林大学化学学院,长春130012
  • 相关基金:国家自然科学基金(No.21571075,21320102001,21621001)、国家重大研发计划(No.2016YFB0701100)和高等学校学科创新引智计划fNo.B17020)资助项目.
中文摘要:

以二丙胺异构体(二正丙胺DPA和二异丙胺D-iPA)为结构导向剂,在200℃加热2组反应原料物质的量之比不同的初始凝胶.合成出了高结晶度的磷酸铝分子筛A1PO4-11。利用X射线粉末衍射分析、元素分析等表征手段,研究了凝胶的晶化过程和液相的pH值以及A1和P的浓度演化。初始凝胶各组分物质的量之比为nAl2O5:nP2O5:nDPA/D:nH2O=1.0:1.0:1.2:75时,以为DPA结构导向剂.晶化过程中无中间相生成,而以D-iPA为结构导向剂时,晶化过程中生成了具有12元环孔道结构的磷酸铝分子筛A1PO4-5中间相;初始凝胶各组分物质的量之比为nAl2O5:nP2O5:nDPA/D:nH2O=1.0:1.0:1.2:75时,以为结构导向剂,晶化过程中DPA生成了具有18元环孔道结构的磷酸铝分子筛VPI-5中间相,而以D-iPA为结构导向剂时,晶化过程中同时出现了VPI-5及A1PO4-5两种中间相。表明对于同一种有机胺,凝胶物质的量之比的改变影响了其结构导向效应。理论计算结果显示质子化的DPA及D-iPA中N原子上的电荷有差异.表明有机胺的结构微调影响其结构导向效应,但该影响依赖于凝胶组成。

英文摘要:

The structure-directing effect of dipropylamine isomers, i.e., di-n-propylamine (DPA) and diisopro- pylamine (D-iPA), was investigated. By heating the initial gels with certain composition at 200 ℃ for 24 h, highly crystalline aluminophosphate molecular sieve A1PO4-11 was obtained. The crystallization processes were investigated using X-ray diffraction, elemental analysis and pH value measurement. For the crystallization process of the initial gel with nA12O3:np205/nDPA/D.iPA :nH2O=l.0:l.0:1.2:75, no intermediate phase was formed when the DPA was used as the structure-directing agent, whereas intermediate phase of aluminophosphate molecular sieve A1PO4-5 was observed when the D-iPA was used as the structure-directing agent. For the crystallization process of the initial gel with nAl2O3 :nP2O5:nDPA/D-iPA :nH2O =1.0:1.0:1.0:75, intermediate phase of aluminophosphate molecular sieve VPI-5 was formed when the DPA was used as the structure-directing agent, whereas intermediate phases of both VPI-5 and A1PO4-5 were observed when the D-iPA was used as the structure-directing agent. Theoretical calculation showed that the charge on the N of the protonated DPA was different with that on the N of the protonated D-iPA. The results indicate that the structure-directing effect of amine can be affected by the composition of the initial gel and the fine-tuning of the structure of amine can influence its structure-directing effect. However, such influence is affected by the composition of the initial gel.

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期刊信息
  • 《无机化学学报》
  • 中国科技核心期刊
  • 主管单位:中国科学技术协会
  • 主办单位:中国化学会
  • 主编:游效曾
  • 地址:南京市南京大学仙林区化学楼
  • 邮编:210023
  • 邮箱:wjhx@nju.edu.cn
  • 电话:025-89682307
  • 国际标准刊号:ISSN:1001-4861
  • 国内统一刊号:ISSN:32-1185/O6
  • 邮发代号:28-133
  • 获奖情况:
  • 2007年获江苏省优秀期刊奖,2009年获华东地区优秀期刊奖
  • 国内外数据库收录:
  • 美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:19587