铜、钇双金属改性NaY分子筛对吸附脱硫性能研究

发布时间：2018-01-12 19:27

本文关键词：铜、钇双金属改性NaY分子筛对吸附脱硫性能研究　出处：《东北石油大学》2015年硕士论文　论文类型：学位论文

【摘要】：本文采用液相离子交换法成功制备了铜、钇双金属改性吸附剂,并采用X射线粉末衍射(XRD)、比表面积测定(BET)、电感藕合等离子体原子发射光谱分析(ICP-AES)、X射线光电子能谱(XPS)、差热-热重分析(TG-DTA)、吡啶红外光谱(Py-IR)、傅立叶变换红外光谱(FT-IR)、扫描电镜(SEM)等一系列表征手段对所制得的吸附剂进行了表征。通过静态吸附脱硫法研究了焙烧温度、阳离子交换顺序、阳离子交换浓度、Cu/Y摩尔比、离子交换时间、吸附剂质量、吸附时间和吸附温度等制备条件对Cu(I)-Y(III)-Y分子筛吸附剂脱硫性能的影响。得到Cu(I)-Y(III)-Y的最适宜制备条件为:先交换Cu后交换Y离子,离子交换24小时,Cu/Y摩尔比为1,离子交换浓度为0.1 mol·L-1,550oC焙烧;用最优制备条件制备的Cu(I)-Y(III)-Y吸附剂对含有苯并噻吩的模拟油(剂油比为0.01g·mL-1)在50 oC条件下吸附60 min后,苯并噻吩脱硫率达到99%。以含有一定量的硫化物(噻吩和苯并噻吩)以及一定量竞争组分(邻二甲苯、间二甲苯和对二甲苯)的正辛烷溶液为模拟油,测试了吸附剂的吸附脱硫性能。实验结果表明,Cu(I)-Y(III)-Y具有类似于Cu(I)-Y的高硫容特性,Cu(I)-Y(III)-Y对各不同硫化物的吸附能力大小为:苯并噻吩2,5-二甲基噻吩3-甲基噻吩噻吩。Cu(I)-Y(III)-Y还具有类似于Y(III)-Y的高选择性,竞争吸附组分邻二甲苯、间二甲苯和对二甲苯对吸附剂脱硫性能的影响大小顺序为:邻二甲苯间二甲苯对二甲苯。Cu(I)-Y(III)-Y通过π络合(通过Cu+)和S-M键(通过Y3+)两种配位键与硫化物发生作用,使得Cu(I)-Y(III)-Y对硫化物具有良好的选择能力和吸附能力。以苯并噻吩为模型化合物,研究了Cu(I)-Y(III)-Y吸附剂等温吸附和吸附动力学,并计算了热力学参数ΔG和ΔH。结果表明:Cu(I)-Y(III)-Y对苯并噻吩的吸附符合Langmuir模型,其吸附动力学可以用准二级速率方程进行描述,Cu(I)-Y(III)-Y吸附剂的吸附脱硫过程是一个自发的放热过程。
[Abstract]:In this paper, copper and yttrium bimetallic modified adsorbents were successfully prepared by liquid phase ion exchange method. X-ray powder diffraction (XRD) and specific surface area determination (BET) were used for the preparation of copper and yttrium bimetallic adsorbents. Inductively coupled plasma atomic emission spectrometry (ICP-AESU) X-ray photoelectron spectroscopy (XPS), differential thermogravimetric analysis (TG-DTAA), pyridine infrared spectroscopy (Py-IRR). The adsorbents were characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM) and so on. The calcination temperature was studied by static adsorption desulfurization method. Cationic exchange order, cationic exchange concentration, Cu / Y molar ratio, ion exchange time, adsorbent mass. Effects of preparation conditions such as adsorption time and adsorption temperature on desulfurization performance of Cu(I)-Y(III)-Y molecular sieve adsorbent. The optimum preparation conditions of -Y are as follows: first exchange Cu and then exchange Y ion. The molar ratio of Cu / Y is 1 and the ion exchange concentration is 0.1 mol 路L ~ (-1) ~ 550oC. Preparation of Cu(I)-Y(III)-Y adsorbents for simulated oils containing benzothiophene (the ratio of solvent to oil is 0.01g 路ml ~ (-1)). After 60 min adsorption at 50oC. The desulfurization rate of benzothiophene is up to 99. The n-octane solution containing a certain amount of sulfides (thiophene and benzothiophene) and a certain amount of competing components (o-xylene, m-xylene and p-xylene) is used as the simulation oil. The adsorption and desulphurization properties of the adsorbent were tested. The experimental results show that the adsorbent has a high sulfur capacity similar to that of Cu(I)-Y. The adsorption ability of Cu(I)-Y(III)-Y to different sulfides is benzothiophene 2. 5- dimethylthiophene 3-methylthiophene. Cuanili-Y also has high selectivity and competitive adsorption of o-xylene, which is similar to that of YPIII- Y. The order of influence of m-xylene and p-xylene on desulfurization performance of adsorbents is: o-xylene m-xylene p-xylene. Cuanine I- (-Y) III- Y is complexed by 蟺 (via Cu). And S-M bond (through Y3) interact with sulfides. The results showed that Cu(I)-Y(III)-Y had good selectivity and adsorption ability for sulfides. Benzothiophene was used as the model compound. The isothermal adsorption and adsorption kinetics of Cu(I)-Y(III)-Y adsorbent were studied. The thermodynamic parameters 螖 G and 螖 H have been calculated. The results show that the adsorption of benzothiophene to benzothiophene at 1: Cu-I-Y is in accordance with the Langmuir model. The adsorption kinetics can be described as a spontaneous exothermic process by using the quasi second order rate equation.
【学位授予单位】：东北石油大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TQ424;X742

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