王舒君,刘璞生,谢鑫,杜晓辉,高雄厚,刘颖.柠檬酸溶液中NaY分子筛的脱铝行为[J].分子催化,2019,33(4):363-370
柠檬酸溶液中NaY分子筛的脱铝行为
Dealumination Behavior of Zeolite NaY in Citric Acid Solution
投稿时间:2019-07-16  修订日期:2019-07-23
DOI:
中文关键词:  NaY分子筛  柠檬酸  硅铝比  介孔
英文关键词:zeolite NaY  citric acid  silica/alumina ratio  mesopore
基金项目:中国石油重大专项(2016E-0701)
作者单位E-mail
王舒君 西北师范大学 化学化工学院, 甘肃 兰州 730070
中国石油石油化工研究院兰州化工研究中心, 甘肃 兰州 730060 
 
刘璞生 中国石油石油化工研究院兰州化工研究中心, 甘肃 兰州 730060  
谢鑫 中国石油石油化工研究院兰州化工研究中心, 甘肃 兰州 730060  
杜晓辉 中国石油石油化工研究院兰州化工研究中心, 甘肃 兰州 730060  
高雄厚 中国石油石油化工研究院, 北京 100195 gaoxionghou@petrochina.com.cn 
刘颖 西北师范大学 化学化工学院, 甘肃 兰州 730070  
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中文摘要:
      硅铝分子筛有机酸配合脱铝是提高其稳定性、引入介孔的一种重要方法.采用X射线衍射、N2物理吸附、高分辨透射电镜、傅里叶变换红外光谱、27Al和29Si固体魔角自旋核磁共振光谱等方法研究了NaY分子筛柠檬酸脱铝行为.结果表明,柠檬酸浓度对NaY分子筛骨架Al原子的脱出影响尤为显著.反应起始阶段,分子筛骨架铝原子快速脱出,其晶体结构遭到严重破坏.随着反应的进行,分子筛硅铝比和结晶度皆有所增加,表明其骨架结构可能进行了重新排列.75℃下,0.10 mol/L柠檬酸处理2 h的脱铝分子筛样品,与NaY分子筛样品相比,其骨架硅铝比增加了0.6、外表面增加了17 m2·g-1,脱铝同时产生了大量无定形硅.
英文摘要:
      The dealumination of aluminosilicate zeolites by organic acid complexation is of great essence to improve the stability of zeolite and introduce mesopores into microporous zeolite. In this study, the dealumination of zeolite NaY by citric acid complexation is systematically investigated by X-ray diffraction, N2 physical adsorption, high-resolution transmission electron microscopy, Fourier transform infrared spectroscopy, 27Al and 29Si solid magic angle spin nuclear magnetic resonance spectroscopy. The results show that of several factors, the citric acid concentration plays a dominant role in the removal of Al atoms from the skeleton of zeolite NaY. At the initial stage, the crystal structure of zeolite NaY is severely damaged due to high extraction rate by citric acid. As the reaction proceeds, the silica/alumina ratio and relative crystallinity both increase. In contrast with the parent zeolite, the skeleton silica/alumina ratio and external surface area for the zeolite Y treated at 75℃ for 2 hours using 0.10 mol/L citric acid increase by 0.6 mol/mol and 17 m2·g-1, respectively. The massive dealumination by citric acid complexation yields a large number of amorphous silica simultaneously.
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