不同硅鋁比Al-ITQ-13分子篩的甲醇制丙烯反應催化性能
發(fā)布時間:2018-07-09 20:27
本文選題:MTP + Al-ITQ-分子篩��; 參考:《燃料化學學報》2017年11期
【摘要】:采用晶種法直接合成了硅鋁比(SiO_2/Al_2O_3物質的量比)為137、224和309的三種Al-ITQ-13分子篩,并采用粉末X射線衍射(XRD)、掃描電鏡(SEM)、N_2吸附-脫附、固體核磁共振(MAS NMR)和NH_3-程序升溫脫附(NH_3-TPD)等分析方法對不同硅鋁比分子篩進行了表征,并在固定床微型反應評價裝置上,考察了硅鋁比對甲醇轉化制丙烯反應性能的影響。結果表明,不同硅鋁比Al-ITQ-13分子篩呈現(xiàn)出相似的織構性質,酸量及酸強度隨著硅鋁比的升高逐漸下降。硅鋁比對甲醇轉化反應的產物分布存在較大的影響;隨著硅鋁比的升高,氫轉移反應和芳構化反應活性降低,使得乙烯選擇性下降,而丙烯和丁烯的選擇性升高。硅鋁比由137提高到309,丙烯的選擇性(質量分數(shù))由46.04%增加到55.52%,而丙烯/乙烯比由3.39提高到6.57。
[Abstract]:Three kinds of Al-ITQ-13 molecular sieves with SiO2 / AlSn2O3 ratio of 137224 and 309were synthesized by means of crystal seeding method, and were adsorbed and desorbed by powder X-ray diffraction (XRD) and scanning electron microscopy (SEM). The molecular sieves with different Si-Al ratios were characterized by solid nuclear magnetic resonance (MAS NMR) and NH _ 3-TPD. The effect of Si / Al ratio on the reaction performance of methanol to propylene was investigated in a fixed-bed micro-reactor. The results show that Al-ITQ-13 zeolites with different Si-Al ratios exhibit similar texture properties, and the acid content and strength decrease with the increase of Si-Al ratio. With the increase of the ratio of Si to Al, the activity of hydrogen transfer reaction and aromatization decreased, and the selectivity of ethylene decreased, while the selectivity of propylene and butene increased. The ratio of Si to Al was increased from 137 to 309, the selectivity (mass fraction) of propylene increased from 46.04% to 55.522%, and the ratio of propylene to ethylene increased from 3.39 to 6.57.
【作者單位】: 中國石油大學(北京)化學工程學院重質油國家重點實驗室;
【基金】:國家自然科學基金(U1462202) 中國石油大學(北京)科研基金(2462015YQ0309)資助~~
【分類號】:O643.36;TQ221.212
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