聚合离子液体的合成及其吸附脱硫性能

doi:10.16085/j.issn.1000-6613.2021-1963

摘要/Abstract

摘要：

以N-甲基二烯丙基胺与金属酞菁合成的功能化离子液体为单体、硅胶球为载体，在载体表面聚合制备成硅胶球负载的聚合功能化离子液体吸附材料[(NMDA-Pc/Ni²⁺)/SiO₂]。本研究采用红外光谱、X射线衍射、扫描电镜、偏光显微镜对其进行表征。考察了吸附剂在常压室温下对二苯并噻吩（DBT）的吸附脱硫性能。结果表明，(NMDA-Pc/Ni²⁺)/SiO₂的吸附脱硫性能最好。最佳吸附条件为吸附剂用量为1.5g/10mL模型油，吸附时间为20min，DBT的最大吸附量为6.198mg/g。该吸附剂对DBT的吸附行为遵循Freundlich 吸附等温模型和拟二级动力学模型。以甲醇洗涤再生，重复使用5次后，吸附性能没有明显降低。烯烃和芳烃都会影响吸附剂的吸附脱硫效果，但芳烃对DBT选择性吸附的影响小于烯烃。吸附剂对不同的硫化合物也有良好的吸附作用，去除顺序为：二苯并噻吩>苯并噻吩>噻吩。

关键词: 聚合, 离子液体, 吸附, 脱硫, 二苯并噻吩, 二氧化硅

Abstract:

Functionalized ionic liquid monomer was synthesized from N-methyldiallylamine and metal phthalocyanine, and then polymerized on the surface of the carrier(silica gel ball) to prepare a polymeric functionalized ionic liquid as an adsorbent[(NMDA-Pc/Ni²⁺)/SiO₂]. The adsorbent was characterized by infrared spectroscopy, X-ray diffraction analysis, scanning electron microscopy, and polarized light microscope. The adsorption and desulfurization performance of the adsorbent for dibenzothiophene(DBT) at normal pressure and room temperature was investigated. The optimal adsorption conditions were the amount of adsorbent of 1.5g/10mL model oil, and the adsorption time of 20min, under which the maximum adsorption capacity of DBT was 6.198mg/g. The adsorption behavior of the adsorbent to DBT followed the Freundlich adsorption isotherm model and the pseudo-second-order kinetic model. The adsorbent was washed and regenerated with methanol, and the adsorption performance was not significantly reduced after reused for 5 times. Both olefins and aromatics affected the adsorption desulfurization performance of the adsorbent, with the former being more significant. The adsorbent also had a good adsorption for different sulfur compounds, and the removal order was dibenzothiophene>benzothiophene>thiophene.

Key words: polymerization, ionic liquids, adsorption, desulfurization, dibenzothiophene, silicon dioxide

中图分类号:

O647.33

单清雯, 张娟, 王亚娟, 刘文强. 聚合离子液体的合成及其吸附脱硫性能[J]. 化工进展, 2022, 41(8): 4571-4579.

SHAN Qingwen, ZHANG Juan, WANG Yajuan, LIU Wenqiang. Synthesis of polymeric ionic liquid and its performance on adsorption desulfurization[J]. Chemical Industry and Engineering Progress, 2022, 41(8): 4571-4579.

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等温吸附模型	参数	数值
Langmuir	q_m/mg·g^-1	6.198
	K_L	20.156
	R²	0.89416
Freundlich	K_F	0.5048
	1/n	0.581
	R²	0.99632

吸附剂	硫化物种类	脱硫量 /mg·g^-1	参考文献
Ni/ZSM-5	DBT	0.496	［31］
过渡金属化合物负载的硅胶体系	DBT	0.5184	［32］
Ni-Ce/Al₂O₃-SiO₂	DBT	3.97	［33］
Cu(Ⅰ)-Y 分子筛	DBT	4.925	［34］
(NMDA-Pc/Ni²⁺)/SiO₂	DBT	6.196	本实验

模型	参数	数值
拟一级动力学	k₁/min^-1	0.06523
	q_e，cal/mg·g^-1	1.4619
	R²	0.78241
拟二级动力学	k₂/min^-1	0.1063
	q_e，cal/mg·g^-1	4.6081
	R²	0.99416

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