导电高分子复合膜材料及其电化学器件
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摘要
导电高分子复合膜材料一般具有优异的电学、力学以及电化学性能，从而在电化学器件,如：驱动器、超级电容器等方面具有重要应用前景。本论文设计和制备了三种聚吡咯复合膜材料，并利用不同的合成与修饰方法有效改善了聚吡咯膜材料的表面粘附性、导电性以及界面相互作用。研制了基于这三种导电高分子复合膜材料的电化学器件。主要研究内容和结果如下：
利用电化学沉积技术制备了聚吡咯/金双层复合膜。在该复合膜表面化学修饰了一层聚多巴胺薄膜，从而有效地提高了其表面生物粘附性。利用聚多巴胺修饰的聚吡咯/金复合膜研制了电化学驱动器。该器件在生理环境中具有良好的驱动性能。同时，通过电化学驱动成功地从大肠杆菌培养液中抓取了大量的大肠杆菌，为在生理环境中富集细菌提供了一种简便的方法。
以石墨烯自支撑膜为工作电极直接电化学沉积聚吡咯，制备了聚吡咯/磺化石墨烯/还原石墨烯的三层复合膜材料。该材料具有类三明治结构，各层之间紧密结合。改善了材料的导电性、力学强度与界面性能。基于该复合膜材料的电化学驱动器，比传统的弯曲型驱动器具有更好的驱动性能。该驱动器在1V电压的驱动下，驱动速率高达158度/秒，循环寿命长达5000次。由于石墨烯的高电导率和低质量密度，从而大幅降低了驱动该器件所需能量。
通过电化学共沉积一步法制备了聚吡咯/磺化石墨烯复合膜材料，为制备石墨烯/导电高分子复合材料提供一种新方法。磺化石墨烯作为导电掺杂剂，均匀分散在聚吡咯体相之中。在气泡模板的控制下，当电沉积电量大于2库伦/平方厘米时，复合膜具有连续多孔结构。利用沉积电量为2库伦/平方厘米复合膜所制备的超级电容器具有高的比电容量（285±8法拉/克），该数值比纯吡咯膜高接近1倍。同时，该超级电容器具有良好的快速充放电性能和循环稳定性。
Composite films of conducting polymers (CP) usually have excellentproperties and multiple functions. Thus, they have potential applications infabricating various electrochemical devices. In this dissertation, three types ofpolypyrrole (PPy) composite films were synthesized through differentstrategies. The conductivity, surface adhesive or mechanical property ofpolypyrrole film has been greatly improved. The electrochemical actuators orsupercapacitors based on these composite films exhibit improved propertiesand functions. The main contents and results are summarized as follows.
A PPy/Au bi-layer composite film was fabricated by electrochemicaldeposition and its surface was modified with a bio-adhesive polymer,polydopamine. The actuator based on the composite film exhibited highperformances of actuation in physiological media. Furthermore, the surface ofthe actuator is sticky in water, and thus can seize bacteria from their aqueoussolutions. Actuation greatly increased the efficiency of adhering bacteria onthe actuator surface, and this technique provides a cheap and convenientapproach for accumulating bacteria from physiological media.
A tri-layer composite film was fabricated by the electrodeposition of PPyonto a sulfonated graphene (SG)/reduced graphene oxide (RGO) bi-layer filmwith sandwich structure. During electrical actuation, PPy and RGO were actedas actuation and conductive inert layers, respectively. The SG layer was usedto enhance the interfacial interactions. The tri-layer actuator exhibited highand stable actuating performance for over1,000actuation cycles, and thelifetime of the actuator was tested to be about5,000cycles. The bending angleof the actuator is larger than360oand its movement rate was higher than150os1under a driving potential of1.0V versus saturated calomel electrode(SCE). Furthermore, the low weight density of graphene based supportinglayer greatly lowered the energy or charge consuming of the actuator duringelectrochemical actuation.
Composite films of sulfonated graphene (SG) and polypyrrole (PPy) wereelectrochemically deposited from the aqueous solutions containing pyrrolemonomer, SG sheets and dodecylbenzene sulfonic acid (DBSA). During theprocess of electrochemical polymerization, negatively charged SG sheetsacted as a dopant of PPy. Thus, they were uniformly dispersed in the PPymatrices of resulting composites. The introduction of SG sheets improved theconductivity and electrochemical properties of PPy films. The supercapacitorbased on the composite films containing about46%(by weight) SG showed ahigh specific capacitance of285F g1at a discharge rate of0.5A g1. Theyalso exhibited greatly improved electrochemical stability and rateperformances.
利用电化学沉积技术制备了聚吡咯/金双层复合膜。在该复合膜表面化学修饰了一层聚多巴胺薄膜，从而有效地提高了其表面生物粘附性。利用聚多巴胺修饰的聚吡咯/金复合膜研制了电化学驱动器。该器件在生理环境中具有良好的驱动性能。同时，通过电化学驱动成功地从大肠杆菌培养液中抓取了大量的大肠杆菌，为在生理环境中富集细菌提供了一种简便的方法。
以石墨烯自支撑膜为工作电极直接电化学沉积聚吡咯，制备了聚吡咯/磺化石墨烯/还原石墨烯的三层复合膜材料。该材料具有类三明治结构，各层之间紧密结合。改善了材料的导电性、力学强度与界面性能。基于该复合膜材料的电化学驱动器，比传统的弯曲型驱动器具有更好的驱动性能。该驱动器在1V电压的驱动下，驱动速率高达158度/秒，循环寿命长达5000次。由于石墨烯的高电导率和低质量密度，从而大幅降低了驱动该器件所需能量。
通过电化学共沉积一步法制备了聚吡咯/磺化石墨烯复合膜材料，为制备石墨烯/导电高分子复合材料提供一种新方法。磺化石墨烯作为导电掺杂剂，均匀分散在聚吡咯体相之中。在气泡模板的控制下，当电沉积电量大于2库伦/平方厘米时，复合膜具有连续多孔结构。利用沉积电量为2库伦/平方厘米复合膜所制备的超级电容器具有高的比电容量（285±8法拉/克），该数值比纯吡咯膜高接近1倍。同时，该超级电容器具有良好的快速充放电性能和循环稳定性。
Composite films of conducting polymers (CP) usually have excellentproperties and multiple functions. Thus, they have potential applications infabricating various electrochemical devices. In this dissertation, three types ofpolypyrrole (PPy) composite films were synthesized through differentstrategies. The conductivity, surface adhesive or mechanical property ofpolypyrrole film has been greatly improved. The electrochemical actuators orsupercapacitors based on these composite films exhibit improved propertiesand functions. The main contents and results are summarized as follows.
A PPy/Au bi-layer composite film was fabricated by electrochemicaldeposition and its surface was modified with a bio-adhesive polymer,polydopamine. The actuator based on the composite film exhibited highperformances of actuation in physiological media. Furthermore, the surface ofthe actuator is sticky in water, and thus can seize bacteria from their aqueoussolutions. Actuation greatly increased the efficiency of adhering bacteria onthe actuator surface, and this technique provides a cheap and convenientapproach for accumulating bacteria from physiological media.
A tri-layer composite film was fabricated by the electrodeposition of PPyonto a sulfonated graphene (SG)/reduced graphene oxide (RGO) bi-layer filmwith sandwich structure. During electrical actuation, PPy and RGO were actedas actuation and conductive inert layers, respectively. The SG layer was usedto enhance the interfacial interactions. The tri-layer actuator exhibited highand stable actuating performance for over1,000actuation cycles, and thelifetime of the actuator was tested to be about5,000cycles. The bending angleof the actuator is larger than360oand its movement rate was higher than150os1under a driving potential of1.0V versus saturated calomel electrode(SCE). Furthermore, the low weight density of graphene based supportinglayer greatly lowered the energy or charge consuming of the actuator duringelectrochemical actuation.
Composite films of sulfonated graphene (SG) and polypyrrole (PPy) wereelectrochemically deposited from the aqueous solutions containing pyrrolemonomer, SG sheets and dodecylbenzene sulfonic acid (DBSA). During theprocess of electrochemical polymerization, negatively charged SG sheetsacted as a dopant of PPy. Thus, they were uniformly dispersed in the PPymatrices of resulting composites. The introduction of SG sheets improved theconductivity and electrochemical properties of PPy films. The supercapacitorbased on the composite films containing about46%(by weight) SG showed ahigh specific capacitance of285F g1at a discharge rate of0.5A g1. Theyalso exhibited greatly improved electrochemical stability and rateperformances.
引文
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