微生物燃料电池新型复合碳电极的制备及其增强产电性能的机制研究

发布时间：2018-03-20 10:52

  本文选题：原位修饰　切入点：石墨烯　出处：《江苏大学》2017年硕士论文　论文类型：学位论文

【摘要】：微生物燃料电池(Microbial fuel cells,MFCs)作为新型节能污水处理技术,能降解有机污染物并直接产生清洁电能,在污水处理、生物传感器、生态修复等领域有巨大的应用潜力。但是,成本高和输出功率低限制了MFCs实际应用。其主要瓶颈是电极材料成本高、制备方法复杂、电化学性能差。因此,开发制备方法简单、性能优异的新型电极成为推进MFCs实际应用的关键。复合碳电极是当前运用最为广泛的电极材料之一,但是存在制备方法复杂、加工耗时长、细胞与电极间作用机制不明确等问题,需要进一步改进和深入研究。本研究采用原位修饰方法分别制备了石墨烯原位修饰(GO)和聚苯胺原位修饰(PANI)的石墨纸复合电极,并开发了一步在石墨纸表面原位同时修饰石墨烯和聚苯胺的新方法,制备获得了石墨烯/聚苯胺修饰的复合石墨纸电极(GO/PANIOS)。本研究进一步对材料特性及其在MFCs中的产电性能进行了研究,并阐明了新型复合碳电极对MFCs产电性能的增强机制。研究结果总结如下:1)采用简单的电化学方法(外加10V直流电压)在石墨纸电极(GP)表面成功快速(4分钟)剥离形成石墨烯层,制备获得了GO电极。通过对MFCs性能比较发现,以GO电极为阳极的MFCs的最大功率密度相比GP电极提高了4.1倍。进一步研究发现,该原位修饰的石墨烯能提高电极的比表面积和润湿性,强化MFCs中产电微生物和电极材料间的直接电子传递过程,进而增强MFCs产电性能。2)采用化学氧化法,对GP电极进行了聚苯胺的缓慢低温原位聚合(12小时),制备了PANIchem电极;采用循环伏安法,以0.1 M硫酸和0.05 M苯胺混合液为电解液,利用三电极体系,在GP电极表面成功原位修饰了聚苯胺(20分钟),制备了PANICV电极。通过对MFCs性能比较研究发现,两种方法修饰的聚苯胺均能增强MFCs产电性能。进一步对MFCs电化学行为进行研究发现,该原位修饰的聚苯胺能提高电极的比表面积,并同步增强MFCs中产电微生物和电极间的直接和间接电子传递过程,进而增强MFCs产电性能。3)基于上述研究发现(原位修饰石墨烯和聚苯胺均能促进MFCs性能),本研究综合改进了石墨烯原位制备和聚苯胺修饰方法,开发了一种一步、原位在石墨纸电极表面快速(4分钟)修饰石墨烯/聚苯胺复合材料的新方法,成功在GP电极表面原位合成了石墨烯/聚苯胺复合材料,制备了GO/PANIOS电极。通过材料表征发现,聚苯胺是以相互交错的纳米丝结构附着于石墨烯上,并以部分氧化和导电状态存在。对相应MFCs性能进行研究发现,以GO/PANIOS电极为阳极MFCs的最大功率密度相比修饰前提高了22倍。进一步对MFCs电化学行为进行研究发现,该原位修饰的石墨烯/聚苯胺复合材料能提高电极比表面积和润湿性,并能协同促进MFCs中产电菌与电极间的直接和间接电子传递过程,进而增强MFCs的产电性能。
[Abstract]:Microbial fuel cells (MFCs), as a new energy-saving sewage treatment technology, can degrade organic pollutants and generate clean electricity directly. It has great application potential in sewage treatment, biosensor, ecological restoration and other fields. High cost and low output power limit the practical application of MFCs. The main bottleneck is the high cost of electrode materials, complex preparation methods and poor electrochemical performance. The new electrode with excellent performance has become the key to promote the practical application of MFCs. The composite carbon electrode is one of the most widely used electrode materials at present, but the preparation method is complex and the processing time is long. In this study, graphene in situ modification (GOG) and Polyaniline (pani) graphite paper composite electrodes were prepared by in situ modification. A new method was developed to modify graphene and Polyaniline simultaneously on the surface of graphite paper. A graphene / Polyaniline modified composite graphite paper electrode was prepared. The properties of the materials and their electrical properties in MFCs were studied. The enhancement mechanism of the new composite carbon electrode on the electrical properties of MFCs was described. The results were summarized as follows: 1) the graphene layer was formed by simple electrochemical method (adding 10V DC voltage) on the surface of the graphite paper electrode for 4 minutes. Go electrode was prepared, and the maximum power density of MFCs with go electrode as anode was 4.1 times higher than that of GP electrode by comparing the performance of MFCs with go electrode. It was found that the maximum power density of MFCs with go electrode as anode was 4.1 times higher than that of GP electrode. The in situ modified graphene can improve the specific surface area and wettability of the electrode, enhance the direct electron transfer process between the electroproducing microorganisms and the electrode materials in MFCs, and then enhance the electrical properties of MFCs. The PANIchem electrode was prepared by slow low temperature in situ polymerization of Polyaniline on GP electrode for 12 hours, and the three-electrode system was used by cyclic voltammetry with a mixture of 0. 1 M sulfuric acid and 0. 05 M aniline as electrolyte. The PANICV electrode was prepared by in situ modification of Polyaniline on the surface of GP electrode for 20 minutes. By comparing the properties of MFCs, it was found that both modified Polyaniline could enhance the electrical properties of MFCs. Furthermore, the electrochemical behavior of MFCs was studied. The in situ modification of Polyaniline can increase the specific surface area of the electrode and synchronously enhance the direct and indirect electron transfer process between the electroproducing microorganisms and the electrode in MFCs. Based on the findings above, both in situ modification of graphene and Polyaniline can promote the performance of MFCs. In this study, a new method of in situ preparation of graphene and modification of Polyaniline was developed by improving the method of in situ preparation of graphene and modification of Polyaniline. The graphene / Polyaniline composite was successfully synthesized on the surface of GP electrode by in situ modification of graphene / Polyaniline composite on the surface of graphite paper electrode for 4 minutes. The GO/PANIOS electrode was prepared. Polyaniline was attached to graphene with interlaced nanowires and existed in partial oxidation and conductive state. The properties of the corresponding MFCs were studied. The maximum power density of MFCs at GO/PANIOS electrode was 22 times higher than that before modification. The electrochemical behavior of MFCs was further studied. It was found that the in situ modified graphene / Polyaniline composite could improve the specific surface area and wettability of the electrode. It can promote the direct and indirect electron transfer process between the electroproducing bacteria and the electrode in MFCs, and then enhance the electrical properties of MFCs.
【学位授予单位】：江苏大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O646.54;TM911.45

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