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低水体系合成X型分子筛及其硅/铝比与碱度的定量关系

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采用不同含水量(n(H2O)/n(SiO2))和碱度(n(M2O)/n(H2O),M为K和Na)的钾-钠体系水热合成X型分子筛,采用X射线荧光光谱、X射线衍射、扫描电镜、29Si魔角旋转固体核磁和27Al魔角旋转固体核磁等手段对X型分子筛进行表征,并对Ba2+交换X型分子筛进行混合碳八芳烃静态吸附评价.结果表明:当合成体系n(SiO2)/n(Al2O3)为2.8时,随着n(H2O)/n(SiO2)从21增加到60,获得纯相X型分子筛的n(M2O)/n(SiO2)范围从1.3逐渐增大至3.1.保持合成体系n(SiO2)/n(Al2O3)不变,X型分子筛n(SiO2)/n(Al2O3)与单一影响因素n(M2O)/n(H2O)线性相关,相关性系数R2为0.90.当合成体系n(SiO2)/n(Al2O3)和n(M2O)/n(H2O)相同时,n(H2O)/n(SiO2)分别为40和60制备的X型分子筛的粒径、非骨架铝物种、孔体积无明显差别.相比而言,低水体系所得X型分子筛的晶体结构中Si(4Al)物种占比更高,对二甲苯相对于乙苯吸附选择性更高,为3.19;对二甲苯相对于邻二甲苯和间二甲苯吸附选择性稍低,分别为3.25和6.84.
Synthesis of X-Type Zeolite in Low Water Content System and Quantitative Relationship Between SiO2/Al2O3 Ratio and Alkalinity
The X-type zeolites were hydrothermally synthesized in the potassium-sodium systems of different water contents(n(H2O)/n(SiO2))and alkalinity(n(M2O)/n(H2O),M represents K and Na).The X-type zeolites were characterized using X-ray fluorescence spectrum,X-ray diffraction,scanning electron microscope,29Si MAS NMR and 27Al MAS NMR.Moreover,an evaluation was performed on the static adsorption of mixed C8 aromatics over Ba2+exchanged X-type zeolites.The results show that when n(SiO2)/n(Al2O3)is 2.8,the n(M2 O)/n(SiO2)range of the obtained pure phase X-type zeolites increases from 1.3 to 3.1 with the increase of n(H2O)/n(SiO2)from 21 to 60.When the n(SiO2)/n(Al2O3)of the synthetic system remains unchanged,the n(SiO2)/n(Al2O3)of X-type zeolite is linearly correlated with the single influencing factor n(M2O)/n(H2O),and the correlation coefficient R2 of 0.90.When n(SiO2)/n(Al2O3)and n(M2O)/n(H2O)are the same,there is no significant difference in particle size,non-skeleton aluminum species and pore volume of X-type zeolites prepared by n(H2O)/n(SiO2)of 40 and 60,respectively.In contrast,the crystal structure of X-type zeolite obtained from the low water system has a higher proportion of Si(4Al)species,and the adsorption selectivity of p-xylene to ethylbenzene is higher(3.19),and the adsorption selectivity of p-xylene to o-xylene and m-xylene is lowered to 3.25 and 6.84,respectively.

FAU topologyX-type zeoliteadsorptive separationp-xylenelow water content

张坚、高宁宁、钟进、王辉国

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中石化石油化工科学研究院有限公司,北京 100083

FAU拓扑结构 X型分子筛 吸附分离 对二甲苯 低含水量

中国石油化工股份有限公司科研开发课题

421108-2

2024

石油学报(石油加工)
中国石油学会

石油学报(石油加工)

CSTPCD北大核心
影响因子:0.764
ISSN:1001-8719
年,卷(期):2024.40(2)
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