稻壳基高纯度NaP1沸石的制备及其庚烷异构性能评价
Preparation of Rice Husk-Based High-Purity NaP1 Zeolite and Evaluation of Heptane Isomerization Performance
作者单位E-mail
张洋 东北石油大学化学化工学院, 大庆 163318  
崔艳红 东北石油大学化学化工学院, 大庆 163318  
马守涛 东北石油大学化学化工学院, 大庆 163318
中国石油大庆化工研究中心, 大庆 163714 
 
张微 东北石油大学化学化工学院, 大庆 163318  
魏媛媛 东北石油大学化学化工学院, 大庆 163318  
所艳华 东北石油大学化学化工学院, 大庆 163318 33367123@qq.com 
摘要: 以稻壳为硅源采用煅烧-水热法合成NaP1沸石,考察了不同硅铝比(nSiO2/nAl2O3)、水钠比(nH2O/nNa2O)、晶化温度、晶化时间对沸石结晶度的影响,并以其为载体制备x% Ni/NaP1(x%为Ni与NaP1的质量比)型烷烃异构催化剂。采用X射线衍射、红外光谱、扫描电子显微镜、透射电子显微镜-X射线能谱、N2气吸附-脱附、X射线光电子能谱、NH3程序升温脱附、差热分析表征手段对合成材料的晶体结构、微观形貌和金属分散性等进行分析,研究了金属镍掺杂对NaP1酸性和热稳定性能的影响。结果表明以稻壳为硅源制备的NaP1沸石的最佳合成条件为水钠比为35、硅铝比为10、晶化温度为95℃、晶化时间为12 h,此时NaP1晶体的结晶度为99.38%。在以正庚烷异构反应为探针的实验中,4% Ni/NaP1的催化性能最佳,在还原温度400℃、还原时间4 h、重时空速3.52 h-1、反应温度为320℃的条件下,收率最大为46.41%,对正庚烷转化率和选择性分别为65.49%和70.86%。
关键词: 稻壳  沸石  水热合成  异构化  多孔材料
基金项目: 东北石油大学国家基金培育基金(No.2017PYYL-03)资助。
Abstract: NaP1 zeolite were synthesized by calcination-hydrothermal method using rice husk as the silicon source. The effects of different silicon-to-aluminum molar ratio (nSiO2/nAl2O3), water-to-sodium molar ratio (nH2O/nNa2O), crystallization temperature and crystallization time on the crystallinity of zeolite were investigated. The alkane isomerization catalyst of x%Ni/NaP1 (x% was the mass ratio of Ni to NaP1) was prepared with the NaP1 zeolite as the support. Xray powder diffraction, infrared spectroscopy, scanning electron microscope, transmission electron microscope-Xray energy spectrum, N2 adsorption-desorption, X-ray photoelectron energy spectrum, NH3 temperature programmed desorption and differential thermal analysis characterization methods were used to analyze the crystal structure, microscopic morphology and metal dispersion of the synthesized materials, and the effect of nickel loading on the acidity and thermal stability of NaP1 were studied. The results showed that the optimal synthesis conditions for NaP1 zeolite prepared from rice husk as silicon source were as follows:nH2O/nNa2O=35, nSiO2/nAl2O3=10, crystallization temperature was 95℃, and the crystallization time was 12 h. Under these synthesizing conditions, the crystallinity of NaP1 crystal was 99.38%. In the experiment of n-heptane isomerization as a probe, 4%Ni/NaP1 had the best catalytic performance at a reduction temperature of 400℃, reduction time of 4 h, weight hourly space velocity of 3.52 h-1, and reaction temperature of 320℃, and the maximum yield was 46.41%, with the conversion of n-heptane and selectivity of iso-heptane of 65.49% and 70.86%, respectively.
Keywords: rice husk  zeolites  hydrothermal synthesis  isomerization  porous materials
投稿时间:2021-03-17 修订日期:2021-06-17
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张洋,崔艳红,马守涛,张微,魏媛媛,所艳华.稻壳基高纯度NaP1沸石的制备及其庚烷异构性能评价[J].无机化学学报,2021,37(9):1613-1624.
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