金属基离子液体负载化SBA-15的合成及其脱硫性能的研究
发布时间：2018-11-06 19:21
【摘要】：随着全球环境污染加剧,世界各国相继实施了一系列更为严格的环境保护法规,尤其是对油品中硫化物含量的要求日益严格。油品中的硫化物经过燃烧以后产生的SOx会导致酸雨、温室效应和空气污染,带来严重的环境问题,所以有效地脱除油品中的硫化物势在必行。催化加氢方法可以有效除去油品中的硫醇、硫醚和二硫化物,但由于噻吩及其衍生物空间位阻效应,传统催化加氢方法对其脱除效果不佳。鉴于离子液体和金属离子都能与噻吩类硫化物发生相互作用,可以在较温和条件下表现出较理想的脱硫效果,所以本文以SBA-15为载体,将离子液体和金属离子共同负载于SBA-15上,在“双活性中心”的作用下进行油品的脱硫,这为吸附脱硫剂的设计与合成供了一个新的思路。本文首先合成离子液体1-乙氧基硅丙基-3-甲基咪唑氯盐(IL),然后分别用溶胶凝胶法和分步法,将离子液体和金属离子共同负载于介孔材料SBA-15上,合成金属基离子液体负载化的SBA-15。将合成的一系列样品使用红外光谱(IR)、X-射线衍射(XRD)、N2吸附脱附、元素分析、扫描电镜(SEM)、能谱分析(EDS)、X-射线荧光(XRF)、原子吸收(AAS)进行表征,结果显示离子液体和金属离子可以共同负载到SBA-15上,并且在一定的比例范围内,负载化的SBA-15仍保持二维六方介孔结构。以溶胶凝胶法合成的一系列负载化SBA-15为吸附剂,对模拟油品进行静态脱硫,筛选最佳吸附剂。实验结果表明,3.2系列的负载化SBA-15对噻吩类硫化物脱除效率最高;对于不同硫化物的脱除效果为:DBTBTTS2-MTS;对于每种吸附剂而言,Zn-IL-SBA-15IL-SBA-15SBA-15。用3.2系列的吸附剂对含不同硫化物的模拟油品进行静态和动态脱硫的实验考察。实验结果表明,在静态脱硫实验中,时间、温度、剂油比对脱硫效率均有一定的影响;动态脱硫实验条件下,Zn-3.2IL-SBA-15对2-甲基噻吩、噻吩、苯并噻吩和二苯并噻吩的穿透时间分别为50min、110min、140min、160min,穿透硫容分别为0.362%、1.667%、2.070%、3.687%。回收实验显示该吸附剂的回收次数不高,有待进一步改进。以溶胶凝胶法合成的Zn-3.2IL-SBA-15为吸附剂,进行脱硫的吸附平衡实验,探究其热力学过程。Zn-3.2IL-SBA-15对噻吩、苯并噻吩的吸附等温线用Henry、Langmuir、Freundlich三种方程进行拟合,实验数据对Langmuir等温方程的拟合效果最好,说明噻吩和苯并噻吩倾向于单分子层吸附。热力学计算结果表明,吸附剂Zn-3.2IL-SBA-15对噻吩和苯并噻吩的吸附过程是自发的、体系混乱度降低、放热的物理过程,噻吩和苯并噻吩分子都属于平行吸附。Zn-3.2IL-SBA-15和硫化物之间存在的π络合、π-π络合和静电吸引力是该吸附剂脱除噻吩类硫化物的内在机理。采用分步法合成金属基离子液体负载化SBA-15,以提高两种活性中心的负载率。实验结果表明,采用分步法虽然可以提高金属离子或者离子液体的负载率,但是脱硫效果提升不高,且易造成SBA-15介孔结构的破坏,其合适的比例,有待进一步探究。
[Abstract]:With the increase of global environmental pollution, the countries of the world have successively implemented a series of more stringent environmental protection regulations, especially the demand for sulfide content in oil products. The SOx produced by the sulfide in the oil can lead to acid rain, greenhouse effect and air pollution, which brings serious environmental problems, so it is imperative to remove the sulfide in the oil effectively. the catalytic hydrogenation method can effectively remove the mercaptans, the thioethers and the disulfides in the oil products, but the traditional catalytic hydrogenation method is not good for the removal effect due to the steric hindrance effect of the alicyclic and the derivatives thereof. in that light of the interaction of the ionic liquid and the metal ion with the sulfur-like sulfide, the ideal desulfurization effect can be exhibited under mild conditions, so that the SBA-15 is used as a carrier, and the ionic liquid and the metal ion are co-loaded on the SBA-15, The desulfurization of oil is carried out under the action of the 鈥渄ouble active center鈥，
本文编号：2315228
[Abstract]:With the increase of global environmental pollution, the countries of the world have successively implemented a series of more stringent environmental protection regulations, especially the demand for sulfide content in oil products. The SOx produced by the sulfide in the oil can lead to acid rain, greenhouse effect and air pollution, which brings serious environmental problems, so it is imperative to remove the sulfide in the oil effectively. the catalytic hydrogenation method can effectively remove the mercaptans, the thioethers and the disulfides in the oil products, but the traditional catalytic hydrogenation method is not good for the removal effect due to the steric hindrance effect of the alicyclic and the derivatives thereof. in that light of the interaction of the ionic liquid and the metal ion with the sulfur-like sulfide, the ideal desulfurization effect can be exhibited under mild conditions, so that the SBA-15 is used as a carrier, and the ionic liquid and the metal ion are co-loaded on the SBA-15, The desulfurization of oil is carried out under the action of the 鈥渄ouble active center鈥，
本文编号：2315228
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