新型纳米级Cu基催化剂的合成及性能研究

发布时间：2018-04-23 21:35

  本文选题：CO + 甲醇　； 参考：《西安石油大学》2017年硕士论文

【摘要】：甲醇是重要的有机化工原料以及C1化学的基础物质,在有机合成、染料、农药、涂料及国防等工业领域被广泛应用。近几年在科学技术的不断发展下,甲醇的用途拓展迅猛,并且逐渐成为一种潜在的车用燃料以及电池燃料。我国的能源特点是富煤、缺油,一次能源以煤为主的格局将长期延续下去,汽、柴油等液体燃料的短缺现象将日趋严重,发展替代燃料特别是煤基洁净替代燃料势在必行,而大力发展煤基醇类(主要是甲醇)代用燃料在中国是完全合乎国情、现实可行的。上世纪60年代以来,合成甲醇催化剂在国内外的研究领域受到重视,虽然从合成气出发合成甲醇已经实现工业化,但相较于国外研究而言,国内Cu基催化剂还存在较大差距。本文结合反应机理、反应热力学和动力学研究了不同组分、制备参数对CO催化加氢制备甲醇的影响,采用共沉淀法制备不同Cu含量、Zn/Al比、助剂Mn含量的催化剂样品,采用微型固定床反应器对其进行活性评价,与催化剂样品的XRD、BET、H_2-TPR、NH3-TPD、SEM、TEM、FTIR等表征结果进行关联,确定当催化剂Cu:Zn:Al:Mn摩尔比为1:2:2:0.05,经复频超声(低频22kHz、高频40kHz)处理,溶液浓度为1.5mol/L,pH为7.5,焙烧温度为550℃、焙烧时间为7h时,催化剂活性较优。实验结合CO加氢反应动力学及热力学,确定反应工艺的主要影响因素为反应压力、反应温度、空速及H_2/CO,通过对筛选的活性及选择性较优催化剂进行活性评价,确定优化反应条件为:反应温度250℃,反应压力6.0MPa,H_2/CO比2.5,液时空速5000h-1,在该反应条件下,CO转化率达到98.50%,甲醇选择性可达到96.51%,并且催化剂性能稳定,使用寿命较长。
[Abstract]:Methanol is an important organic chemical raw material and basic material of C1 chemistry. It is widely used in organic synthesis, dyes, pesticides, coatings and national defense industries. In recent years, with the development of science and technology, the use of methanol has expanded rapidly, and gradually become a potential fuel for vehicles and fuel cells. The energy characteristics of our country are rich in coal and lack of oil. The pattern of primary energy based on coal will continue for a long time. The shortage of liquid fuels such as steam and diesel will become more and more serious. It is imperative to develop alternative fuels, especially coal based clean alternative fuels. The development of coal-based alcohols (mainly methanol) substitute fuels in China is fully in line with the national conditions and practical. Since the 1960s, methanol synthesis catalysts have been paid more attention in the domestic and foreign research fields. Although methanol synthesis from syngas has been industrialized, there is still a big gap between domestic and foreign research. Based on the reaction mechanism, thermodynamics and kinetics, the effects of different components and preparation parameters on the catalytic hydrogenation of CO to methanol were studied in this paper. The samples of different Cu content Zn / Al ratio and mn content of auxiliaries were prepared by coprecipitation method. The microscale fixed-bed reactor was used to evaluate its activity, which was correlated with the characterization results of XRDD-BETH _ 2-TPR-NH _ 3-TPD _ 3-TPDH _ (TM) T _ (TM) T _ (T) IR. It was determined that when the molar ratio of catalyst Cu:Zn:Al:Mn was 1: 2: 2: 0.05, the catalyst was treated by complex frequency ultrasound (low frequency 22 kHz, high frequency 40 kHz). When the solution concentration was 1.5 mol / L, pH was 7.5, calcination temperature was 550 鈩，

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