新型石墨纸和石墨烯在微生物燃料电池中的应用研究
摘要
微生物燃料电池（microbial fuel cells，MFCs）是一种利用自然界中廉价易得的微生物细菌作为生物催化剂，将有机物中的化学能转变为电能的装置。在废水处理、植入式医疗设备和生物传感器等方面有巨大的潜在应用价值。但是微生物燃料电池的输出功率密度偏低，限制了其大规模的实际应用。影响微生物燃料电池性能的因素有：电池构型、接种体、培养基、质子交换材料和电极面积等，其中阴阳极材料是影响其性能的主要因素。阳极材料决定着细菌的实际附着量和界面电子传递电阻的大小。因此，一个高效能的阳极材料对于提高微生物燃料电池的功率输出起着十分重要的作用。在阴极，氧气因其在环境中方便易得并且产物干净环保，是一种理想的阴极电子受体。但是在微生物燃料电池的阴极介质中，氧还原反应的动力学过程较差，从而限制了其作为阴极最终电子受体的使用，因此需要寻找高效的氧还原催化剂。
本论文将新型石墨纸（novel graphite paper，GTS）和石墨烯（graphene）应用于微生物燃料电池，解决微生物燃料电池阳极和阴极中存在的问题，提高电池的功率密度，改善电池的产电性能。具体来说本论文的研究结果概括如下：
（1）以大肠杆菌（E.coli）为生物催化剂，GTS为阳极构建双室型微生物燃料电池，放电曲线和极化曲线显示：GTS有很好的电催化性能。该电池的最大输出功率密度为2249mW m~(-2)。从扫描电镜（scanning electron microscopy，SEM）结果来看，这可能归因于GTS良好的生物兼容性。
（2）以聚四氟乙烯（polytetrafluoroethylene，PTFE）为粘合剂，不锈钢网（stainlesssteel mesh，SSM）为基底，附载石墨烯作为阳极构建微生物燃料电池。SSM电极、 PTFE修饰的SSM电极（PMS）和石墨烯修饰的SSM电极（GMS）的循环伏安（cyclicvoltammogram，CV）、放电曲线和极化曲线结果显示：GMS的电化学性能最好。以GMS为阳极构建的微生物燃料电池的最大功率密度可达2668mW m~(-2)，分别比以SSM和PMS为阳极的电池功率大18和17倍。
（3）利用透射电镜（transmission electron microscopy，TEM）和X射线光电子能谱（X-ray photoelectron spectroscopy，XPS）分别对石墨烯的形貌和元素组成进行了表征。循环伏安的测定结果显示：石墨烯在中性的缓冲溶液中对氧气的还原反应具有较好的催化活性。以不锈钢网附载石墨烯作为阴极可以提高微生物燃料电池的产电性能，最大功率密度为289mW m~(-2)。
（4）利用非共价方法制备四磺酸基酞菁铁（iron tetrasulfophthalocyanine，FeTsPc）修饰的石墨烯复合物（FeTsPc-graphene），该方法可以在防止石墨烯团聚的同时，生成一种有效的氧还原催化剂。利用循环伏安法和线性扫描伏安法（linear sweepvoltammogram，LSV）对FeTsPc-graphene进行了电化学测试，发现其比FeTsPc修饰的电极的氧还原电位更正，电流更大。将FeTsPc-graphene修饰的碳纸用作微生物燃料电池的阴极，电池功率可达817mW m~(-2)，要大于用FeTsPc修饰的电极结果（523mW m~(-2)），与用铂/碳（Pt/C）修饰的电极结果（856mW m~(-2)）相似，因此，在微生物燃料电池中，FeTsPc-graphene复合物可以替代铂用于催化氧的还原。
Microbial fuel cells (MFCs) are renewable energy devices that can convert organicsubstrates into electricity via the catalyzation of microorganisms. The low power density ofMFCs remains one of the main obstacles for their practical applications. Aside from all theother factors affecting the MFCs performance, which include cell design, inoculum, substrate,proton exchange material and electrode surface areas, etc. the fabrication materials of anodeand cathode play a profound role in influencing the power generation. The anode material candetermine the actual accessible area for bacteria to anchor and affect the interfacial electrontransfer resistance. Therefore, a high-performance anode material is most essential to improvethe power outputs of MFCs. In cathode, oxygen is an ideal electron acceptor due to itsaccessibility in environment and clean product. However, the poor kinetics of oxygenreduction reaction in the MFCs cathodic medium limits the efficient utilization of oxygen asfinal electron acceptor for most cathode materials.
In this study, novel graphite paper (GTS) and graphene were used to improve theperformance of MFCs. Some innovative findings have been found as follows:
(1) GTS has been used as anodic catalyst in MFC based on E.coli (ATCC25922) andcharacterized by discharge experiment and polarization curve. Findings from thesemeasurements revealed that GTS showed an excellent electrochemical performance. Thetwo-chambered MFC operated with the GTS anode delivered a maximum power density of2249mW m~(-2). Scanning electron microscopy (SEM) results indicate that the high poweroutput could be attributed to the high biocompatibility of the GTS.
(2) A graphene-modified stainless steel mesh (GMS) has been used as anodic catalyst ofMFCs based on E.coli. The electrochemical activities of stainless steel mesh (SSM),polytetrafluoroethylene (PTFE) modified SSM (PMS) and GMS have been investigated bycyclic voltammogram (CV), discharge experiment and polarization curve measurement. TheGMS shows better electrochemical performance than those of SSM and PMS. The MFCequipped with GMS anode delivers a maximum power density of2668mW m~(-2), which is18times larger than that obtained from the MFC with the SSM anode and is17times larger thanthat obtained from the MFC with the PMS anode.
(3) The morphologies and surface elemental analysis of graphene were characterized bytransmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Theelectrochemical activity was evaluated by CV. Graphene exhibited high oxygen reductionactivity. The MFC operated with the graphene cathode delivered a maximum power density of 289mW m~(-2), which demonstrated that the graphene is promising candidate for application ofMFC.
(4) Noncovalent functionalization of graphene with iron tetrasulfophthalocyanine(FeTsPc) is achieved not only to prevent the aggregation of graphene but also form anefficient electrocatalyst for the oxygen reduction reaction (ORR) in a dual-chamber microbialfuel cell. The electrochemical activity of the FeTsPc-functionalized graphene(FeTsPc-graphene) is evaluated towards the ORR using CV and linear sweep voltammogram(LSV) methods. More positive peak potential and larger peak current of oxygen reduction arefound using FeTsPc-graphene electrode as compared to FeTsPc electrode. The maximumpower density of817mW m~(-2)obtained from the MFC with a FeTsPc-graphene cathode ishigher than that of523mW m~(-2)with a FeTsPc cathode and is close to that of856mW m~(-2)with a Pt/C cathode. Thus, FeTsPc-graphene nanocomposites can be a good alternative to Ptcatalyst in MFCs.
本论文将新型石墨纸（novel graphite paper，GTS）和石墨烯（graphene）应用于微生物燃料电池，解决微生物燃料电池阳极和阴极中存在的问题，提高电池的功率密度，改善电池的产电性能。具体来说本论文的研究结果概括如下：
（1）以大肠杆菌（E.coli）为生物催化剂，GTS为阳极构建双室型微生物燃料电池，放电曲线和极化曲线显示：GTS有很好的电催化性能。该电池的最大输出功率密度为2249mW m~(-2)。从扫描电镜（scanning electron microscopy，SEM）结果来看，这可能归因于GTS良好的生物兼容性。
（2）以聚四氟乙烯（polytetrafluoroethylene，PTFE）为粘合剂，不锈钢网（stainlesssteel mesh，SSM）为基底，附载石墨烯作为阳极构建微生物燃料电池。SSM电极、 PTFE修饰的SSM电极（PMS）和石墨烯修饰的SSM电极（GMS）的循环伏安（cyclicvoltammogram，CV）、放电曲线和极化曲线结果显示：GMS的电化学性能最好。以GMS为阳极构建的微生物燃料电池的最大功率密度可达2668mW m~(-2)，分别比以SSM和PMS为阳极的电池功率大18和17倍。
（3）利用透射电镜（transmission electron microscopy，TEM）和X射线光电子能谱（X-ray photoelectron spectroscopy，XPS）分别对石墨烯的形貌和元素组成进行了表征。循环伏安的测定结果显示：石墨烯在中性的缓冲溶液中对氧气的还原反应具有较好的催化活性。以不锈钢网附载石墨烯作为阴极可以提高微生物燃料电池的产电性能，最大功率密度为289mW m~(-2)。
（4）利用非共价方法制备四磺酸基酞菁铁（iron tetrasulfophthalocyanine，FeTsPc）修饰的石墨烯复合物（FeTsPc-graphene），该方法可以在防止石墨烯团聚的同时，生成一种有效的氧还原催化剂。利用循环伏安法和线性扫描伏安法（linear sweepvoltammogram，LSV）对FeTsPc-graphene进行了电化学测试，发现其比FeTsPc修饰的电极的氧还原电位更正，电流更大。将FeTsPc-graphene修饰的碳纸用作微生物燃料电池的阴极，电池功率可达817mW m~(-2)，要大于用FeTsPc修饰的电极结果（523mW m~(-2)），与用铂/碳（Pt/C）修饰的电极结果（856mW m~(-2)）相似，因此，在微生物燃料电池中，FeTsPc-graphene复合物可以替代铂用于催化氧的还原。
Microbial fuel cells (MFCs) are renewable energy devices that can convert organicsubstrates into electricity via the catalyzation of microorganisms. The low power density ofMFCs remains one of the main obstacles for their practical applications. Aside from all theother factors affecting the MFCs performance, which include cell design, inoculum, substrate,proton exchange material and electrode surface areas, etc. the fabrication materials of anodeand cathode play a profound role in influencing the power generation. The anode material candetermine the actual accessible area for bacteria to anchor and affect the interfacial electrontransfer resistance. Therefore, a high-performance anode material is most essential to improvethe power outputs of MFCs. In cathode, oxygen is an ideal electron acceptor due to itsaccessibility in environment and clean product. However, the poor kinetics of oxygenreduction reaction in the MFCs cathodic medium limits the efficient utilization of oxygen asfinal electron acceptor for most cathode materials.
In this study, novel graphite paper (GTS) and graphene were used to improve theperformance of MFCs. Some innovative findings have been found as follows:
(1) GTS has been used as anodic catalyst in MFC based on E.coli (ATCC25922) andcharacterized by discharge experiment and polarization curve. Findings from thesemeasurements revealed that GTS showed an excellent electrochemical performance. Thetwo-chambered MFC operated with the GTS anode delivered a maximum power density of2249mW m~(-2). Scanning electron microscopy (SEM) results indicate that the high poweroutput could be attributed to the high biocompatibility of the GTS.
(2) A graphene-modified stainless steel mesh (GMS) has been used as anodic catalyst ofMFCs based on E.coli. The electrochemical activities of stainless steel mesh (SSM),polytetrafluoroethylene (PTFE) modified SSM (PMS) and GMS have been investigated bycyclic voltammogram (CV), discharge experiment and polarization curve measurement. TheGMS shows better electrochemical performance than those of SSM and PMS. The MFCequipped with GMS anode delivers a maximum power density of2668mW m~(-2), which is18times larger than that obtained from the MFC with the SSM anode and is17times larger thanthat obtained from the MFC with the PMS anode.
(3) The morphologies and surface elemental analysis of graphene were characterized bytransmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Theelectrochemical activity was evaluated by CV. Graphene exhibited high oxygen reductionactivity. The MFC operated with the graphene cathode delivered a maximum power density of 289mW m~(-2), which demonstrated that the graphene is promising candidate for application ofMFC.
(4) Noncovalent functionalization of graphene with iron tetrasulfophthalocyanine(FeTsPc) is achieved not only to prevent the aggregation of graphene but also form anefficient electrocatalyst for the oxygen reduction reaction (ORR) in a dual-chamber microbialfuel cell. The electrochemical activity of the FeTsPc-functionalized graphene(FeTsPc-graphene) is evaluated towards the ORR using CV and linear sweep voltammogram(LSV) methods. More positive peak potential and larger peak current of oxygen reduction arefound using FeTsPc-graphene electrode as compared to FeTsPc electrode. The maximumpower density of817mW m~(-2)obtained from the MFC with a FeTsPc-graphene cathode ishigher than that of523mW m~(-2)with a FeTsPc cathode and is close to that of856mW m~(-2)with a Pt/C cathode. Thus, FeTsPc-graphene nanocomposites can be a good alternative to Ptcatalyst in MFCs.
引文
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