聚丙烯生物质协同碳化制备碳纳米管基杂化材料及应用研究

发布时间：2018-06-07 00:48

本文选题：聚丙烯 + 生物质　；参考：《东北林业大学》2017年硕士论文

【摘要】：目前,单纯碳纳米管的合成已经比较成熟并在一些领域实现替代传统材料的目的,而对碳纳米管基杂化材料的研究仍处于初级阶段。由于杂化材料通常会体现出介于两种材料之间的优异性能甚至出现新的特性,因此,研究碳纳米管基杂化材料具有重要的研究价值。本论文在一步裂解法催化高聚物合成碳纳米管的基础上,设计合成出稻壳基生物质炭-碳纳米管杂化材料、珊瑚状稻壳基-碳纳米管杂化材料和纤维素接枝碳纳米管的C-C杂化材料这三种新型碳基-碳纳米管纳米杂化材料;并探究了几种新型材料的应用性能。本文通过一步热解PP/Ni-Mo-Mg/Cl-Rice-Char复合材料合成了稻壳基生物质炭-碳纳米管杂化材料。为了表征碳产物的微观结构、相结构、热稳定性和吸附性能,并探讨Cl-Rice-Char与Ni-Mo-Mg的协同机理,分别应用了扫描电子显微镜(SEM),透射电子显微镜(TEM),X射线衍射仪(XRD),拉曼光谱仪(Raman)、热重分析仪(TGA)、氮气吸附-脱附测试、X射线光电子显微镜(XPS)等表征手段。研究结果表明:Cl-Rice-Char在复合材料的热解过程中能与Ni-Mo-Mg催化剂产生协同作用,加速PP的脱氢降解以生成CNTs;同时,能控制NH4Cl的释放速率延长协同性能。当添加5wt% Cl-Rice-Char时,碳产物形貌最佳。吸附试验结果表明,该新型杂化材料的吸附能力高达452.5mg/g。本文利用控制变量法,探究了 Ni2O3/NH4Cl体系协效催化聚丙烯/稻壳共裂解制备生物质基-碳纳米管杂化材料的规律。并采用相应的检测手段,表征与分析了碳产物的微观结构、相结构、热稳定性。结果表明:Ni2O3、NH4Cl、稻壳三者之间,在最佳配比的情况下能够产生协同作用,当复合材料的配比为PP/5%Ni2O3/0.5%NH4Cl/10%稻壳时,一步热解该复合材料能够得到珊瑚状稻壳基-碳纳米管杂化材料。吸附试验结果表明,珊瑚状稻壳基-碳纳米管杂化材料的吸附能力良好。本文还通过Ni-Mo-Mg催化剂,催化热解PP/Cellulose共混物合成了 C-C杂化材料(纤维素接枝碳纳米管杂化材料)。应用多种表征手段,对C-C杂化材料的微观结构、相结构及热稳定性进行了分析。研究结果表明:当各组分比例为PP/5%Ni-Mo-Mg/30%Cellulose时,热解该复合材料可以获得形态最佳的C-C杂化材料。在热解的过程中,聚丙烯仅作为生长碳纳米管的碳源,纤维素仅作为宏观碳基质的前驱体,Ni-Mo-Mg 催化剂的作用是催化聚丙烯脱氢降解并以纤维素碳基质为母体,在缺陷处接枝生长碳纳米管。
[Abstract]:At present, the synthesis of pure carbon nanotubes (CNTs) has been mature and has achieved the purpose of replacing traditional materials in some fields. However, the research of CNTs based hybrid materials is still in the primary stage. Because hybrid materials usually exhibit excellent properties or even new properties between two kinds of materials, it is of great value to study carbon nanotube based hybrid materials. In this paper, based on the synthesis of carbon nanotubes by one-step pyrolysis method, the hybrid materials of rice husk based biomass carbon-carbon nanotubes were designed and synthesized. Coralline rice husk / carbon nanotube hybrid material and cellulose grafted carbon nanotube hybrid material are three new carbon-carbon nanotube hybrid materials, and the application properties of several new materials are studied. In this paper, rice husk based biomass carbon nanotube hybrid materials were synthesized by one step pyrolysis of PP/Ni-Mo-Mg/Cl-Rice-Char composites. In order to characterize the microstructure, phase structure, thermal stability and adsorption properties of carbon products, the synergistic mechanism of Cl-Rice-Char and Ni-Mo-Mg was discussed. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffractometer (XRDX), Raman spectrometer (Ram), thermogravimetric analyzer (TGA), nitrogen adsorption-desorption test (TGA) and X-ray photoelectron microscopy (XPSs) were used. The results show that: Cl-Rice-Char can cooperate with Ni-Mo-Mg catalyst in the pyrolysis process of composites, accelerate the dehydrogenation degradation of PP to form CNTs, and control the release rate of NH4Cl to prolong the synergistic performance. When 5 wt% Cl-Rice-Char was added, the morphology of the carbon product was the best. The adsorption capacity of the new hybrid material is 452.5 mg / g. In this paper, the synergistic effect of Ni2O3/NH4Cl system on the co-cracking of polypropylene / rice husk to produce biomass-based carbon nanotube hybrid materials was studied by the method of controlling variables. The microstructure, phase structure and thermal stability of the carbon products were characterized and analyzed by the corresponding detection methods. The results showed that there could be synergistic effect among the three groups, the proportion of the rice husk was the best ratio. When the ratio of the composite was PP- / 5Ni2O3 / 0.5NH4Cl-10% rice husk, the coral-like rice husk matrix / carbon nanotube hybrid material could be obtained by one step pyrolysis of the composite. The adsorption test results showed that coralline rice husk-carbon nanotube hybrid materials had good adsorption capacity. C-C hybrid material (Cellulose grafted carbon nanotube hybrid material) was also synthesized by catalytic pyrolysis of PP/Cellulose blends over Ni-Mo-Mg catalyst. The microstructure, phase structure and thermal stability of C-C hybrid materials were analyzed by various characterization methods. The results show that the best morphology of C-C hybrid material can be obtained by pyrolysis of the composite when the ratio of each component is PP/5%Ni-Mo-Mg/30 llulose. During pyrolysis, polypropylene was only used as carbon source for growth of carbon nanotubes, and cellulose was used as the precursor of macroscopic carbon matrix, which was used as catalyst for dehydrogenation and degradation of polypropylene, and cellulose carbon matrix was used as matrix. Carbon nanotubes were grown by grafting at defects.
【学位授予单位】：东北林业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TQ127.11;TB33

【参考文献】