基于新型纳米结构超级电容器材料的研究
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摘要
人类对化石能源的过渡依赖和消耗造成了严重的环境问题和能源危机,为实现可持续发展的能源的开发和利用,新能源和新型能源装置研究引起广泛关注。作为一种能量存储装置,超级电容器具有非常高的功率密度、长循环寿命、充放电速度快、对环境无污染等特点。纳米材料的广泛研究极大地推动了超级电容器等先进储能技术的蓬勃发展。然而,超级电容器材料的导电性能差、局部分散不均匀、与电解液接触面性能不稳定等纳米材料领域常见的问题同样关系着超级电容器基本性能。本论文针对超级电容器中出现的这些问题,以提高材料电导率和构建多孔结构提高比表面为出发点,进行电极材料的设计、合成与性能研究。经过材料的复合和结构的调控,包括过渡金属氧化物、导电聚合物与多孔金属之间的复合和一维线状结构、二维纳米多孔结构和三维大孔结构的设计制备,进一步改善超级电容器材料的电容性能。论文的宗旨是调控材料的导电性和导离子的性能,进而可以有效调节超级电容器的性能。本论文介绍的新型结构材料有望在超级电容器上得到应用,同时我们希望文中所述材料可应用于其他领域并对其他材料的结构调控具有指导意义。本论文主要研究内容如下：
1、MnO2/PANI复合材料的控制合成及其电化学电容性能研究
我们通过水溶液/有机溶液界面合成的方法,可控合成了一系列MnO2/PANI复合材料。该材料具有一维连续结构,通过改变溶液的PH值,可以有效的调控材料微观结构和复合材料中MnO2/PANI的含量比例。本工作研究了实验制备复合材料的结构特征和其形成机理。实验结果表明中间产物MnO2在产物结构的形成过程中起着重要的作用。工作还研究了该复合材料在超级电容器方面的性能。结果表明在合适pH下合成的MnO2/PANI复合材料具有最高的电容值207Fg-1,比实验制备的纯MnO2和PANI都要大,且表现出较好的稳定性。该复合材料高的比电容可以归因于PANI的链接和导电剂作用,而具有较好的稳定性,则是因为均匀分散的MnO2具有聚苯胺外壳的保护,从而减弱了在充放电过程中的颗粒团聚。
2、具有高能量和功率密度的全固态薄膜超级电容器的研究
便携式和微型化电子器件的快速发展对与之相匹配的能源转换或存储装置的设计和制造提出了新的挑战。本工作设计制备了纳米多孔金属(纳米多孔金NPG)和导电聚合物(聚吡咯PPy)复合薄膜材料(NPG/PPy), PPy均匀的包覆在NPG的表面,具有典型的金属/导电聚合物核壳结构。双连续的开孔结构,具有优良的导电性和连续的纳米孔道,提高了材料的导离子性能,继而提高了材料的利用效率。该材料用于制备一种超薄的柔性固态超级电容器,此电容器是基于一种固态电解液组装而成,NPG作为衬底材料,可提供高的比表面积和优良的导电性,同时可作为集流器,而固态电解液作为电解液和隔膜,简化了电容器组装过程。该固态柔性超级电容器具有较高的功率和能量密度296kW kg-1和27Wh kg"1,高于之前的所有关于PPy的报道,且具有良好的充放电循环特性和柔韧性,有望在便携式电子器件上得到应用。
3、NPG/金属氧化物薄膜复合材料及其电化学电容性能的研究
我们通过一种简单的电化学方法制备了纳米多孔金(NPG)/过渡金属氧化物(Cox、RuO2)复合材料,氧化物材料具有连续的层状结构并与NPG形成三明治夹心结构。该材料以NPG为结构支撑和集电器,而过渡金属氧化物提供高的比电容,从而提高材料整体电容。实验结果表明,氧化钴的体积和质量比电容分别达到了598F cm-3和563Fg-1,并且该材料表现出优异的稳定性。
虽然许多结构材料可以得到高的质量比电容,但是它们的活性材料载量较低,限制了表观电容的提高。比起质量比电容许多应用领域如小尺寸电子产品或传统能量储存装置显然更在意表观电容量。本工作利用独立支撑的NPG电极作为衬底材料,制备NPG/RuO2复合材料,以期获得较大的表观电容。NPG可同时作为集流器和结构支撑材料,Ru02作为电容活性材料。实验结果表明Ru02的电容高达520Fg-1,NPG/RuO2复合材料的表观电容达到了1.5Fcm-2,并且具有优良的倍率性能和较好的稳定性。
4、MnOx纳米线/大孔金属复合材料及其电化学电容性能研究
超级电容器因具有高的功率密度、长循环寿命和良好的安全性能被广泛应用于混合电动车能源系统、数字远程通信系统、不间断电源、脉冲激光技术等领域。比起质量比电容许多应用领域更在意高的表观电容量。本工作通过水热合成的方法制备了MnOx纳米线/大孔金属复合材料,该材料使用泡沫镍的网状结构为氧化锰纳米线提供良好的导电性,开孔的三维结构可以提供畅通的电解液通道,为离子传输提供方便。相互缠绕堆积的氧化锰纳米线首先依靠相互之间的联系提供赝电容,继而通过三维网状结构基底完成充放电过程。实验结果表明,MnOx质量比电容为576Fg-1,而本实验所得泡沫镍/MnOx样品的表观电容值达到了7.6Fcm-2,且表现出较好的稳定性。
The extensive dependence on fossil fuels has caused significant environmental pollution as well as energy resource crisis. Sustainable exploration and use of energy source depend on discovery of new energy source and development of novel energy devices. As a kind of energy storage device, supercapacitors have many advantages over conventional batteries:high power density, long cycling stability, fast charge-discharge rate and being environment friendly. Wide research of nanoscale materials has promoted flourish of advanced energy storage technology. However, common problems involved with nanomaterials such as bad structural continuity, conglomeration and structural instability have restricted their application in supercapacitors. This work introduces strategies based on design of porous materials with high area aiming at improve the performance of the supercapacitors. We have conducted the design, synthesis and performance research of the electrode materials containing:the composite of porous metal materials with transition metal oxide and conducting polymers, one dimensional structural composite and macroporous metal/metal oxide hybrid materials. We demonstrate the above composite materials have wide prospect for application in the supercapacitors as well as other similar fields.
1. Controllable synthesis of MnO2/polyaniline nanocomposite and its electrochemical capacitive property.
Polyaniline (PANI) and MnO2/PANI composites are simply and controllably fabricated by one-step interfacial polymerization at various pH. The morphologies and components of MnO2/PANI composites are modulated by changing pH of the solution. Formation procedure and capacitive property of the products are investigated by XRD,FTIR, TEM and electrochemical techniques. We demonstrate that MnO2as an intermedia material plays a key role in the formation of sample structures. The MnO2/PANI composites exhibit good cycling stability as well as a high capacitance close to207F g-1. Samples fabricated with the facile one-step method are also expected to be adopted in other field such as catalysis, lithium ion battery and biosensor.
2. Sub-micrometer-thick all-solid-state supercapacitors with high power and energy densities.
Fast development of portable and miniature electrics desires compatible energy conversion and storage devices. A flexible NPG-PPy composite film was fabricated using a convenient dealloying and electro-polymerization process. The bicontinuous pore/ligament structure provides high electric conductivity as well as improved ionic transferring channels, which increases the efficiency of the active materials. All-solid-state supercapacitors were designed with NPG-PPy films as both electrodes and PVA as both the separator and electrolyte. The symmetric supercapacitor thus-produced offers large specific capacitance, power density and energy density (296kW kg-1and27Wh kg-1), and exhibits almost identical performance at various curvatures, which suggests its wide application prospect in powering wearable/miniaturized electronics.
3. Electrochemical capacitive behavior of metal oxide and nanoporous gold hybrid structure.
Cobalt oxide and nanoporous gold (NPG) hybrid films are fabricated by a facile electrochemical technique. Structural morphology, composition and capacitive behavior of the sample have been investigated. The composite film has a sandwich like structure containing NPG film as the inside layer and cobalt oxide films as outside layers. NPG, as a3dimensional interconnected skeleton, can afford electron and ion transfer channels thus improve the efficiency of cobalt oxide. The hybrid films provide high volumetric (598F cm-3) and gravimetric capacitances (563F g-1), additionally exhibit good stibility.
To improve the apparent capacitance of the supercapacitors, we chose the ideal capacitive material RuO2as the active electrode material. NPG/RuO2composites are synthesized by CV method using NPG as the substrate and the corrent collectors. The gravimetric capacitance of RuO2achieves502F g-1, and the volumetric capacitance of the composite is close to1.5F g-1.
4. MnOx Nanowires aligned on the macroporous structures with high volumetric electrochemical capacitance.
Because of their high power densities, long lifespan and safe operation, supercapacitors have been used in the areas of hybrid vehicles, digital telecommunication systems, uninterrupted backup energy systems and pulsed laser techniques. The fast development of electronic techniques such as portable electronics or stationary energy storage devices poses new challenges for the design and fabrication of compatible energy devices with large amount of energy stored per area as well as energy per mass. For this work, we propose a facile hydrothermal synthesis method for MnOx nanowires aligned on Ni foam. As prepared porous nanostructures can provide fast electronic transferring channels and reduce ionic diffusion distance with enlarged electrode/electrolyte contact area. The entangled MnOx nanowires provide high pseudocapacitance, and the porous Ni foam serves as substrate and current collectors. The capacitance per mass and area are estimated as high as576F g-1and7.6F cm-2.
1、MnO2/PANI复合材料的控制合成及其电化学电容性能研究
我们通过水溶液/有机溶液界面合成的方法,可控合成了一系列MnO2/PANI复合材料。该材料具有一维连续结构,通过改变溶液的PH值,可以有效的调控材料微观结构和复合材料中MnO2/PANI的含量比例。本工作研究了实验制备复合材料的结构特征和其形成机理。实验结果表明中间产物MnO2在产物结构的形成过程中起着重要的作用。工作还研究了该复合材料在超级电容器方面的性能。结果表明在合适pH下合成的MnO2/PANI复合材料具有最高的电容值207Fg-1,比实验制备的纯MnO2和PANI都要大,且表现出较好的稳定性。该复合材料高的比电容可以归因于PANI的链接和导电剂作用,而具有较好的稳定性,则是因为均匀分散的MnO2具有聚苯胺外壳的保护,从而减弱了在充放电过程中的颗粒团聚。
2、具有高能量和功率密度的全固态薄膜超级电容器的研究
便携式和微型化电子器件的快速发展对与之相匹配的能源转换或存储装置的设计和制造提出了新的挑战。本工作设计制备了纳米多孔金属(纳米多孔金NPG)和导电聚合物(聚吡咯PPy)复合薄膜材料(NPG/PPy), PPy均匀的包覆在NPG的表面,具有典型的金属/导电聚合物核壳结构。双连续的开孔结构,具有优良的导电性和连续的纳米孔道,提高了材料的导离子性能,继而提高了材料的利用效率。该材料用于制备一种超薄的柔性固态超级电容器,此电容器是基于一种固态电解液组装而成,NPG作为衬底材料,可提供高的比表面积和优良的导电性,同时可作为集流器,而固态电解液作为电解液和隔膜,简化了电容器组装过程。该固态柔性超级电容器具有较高的功率和能量密度296kW kg-1和27Wh kg"1,高于之前的所有关于PPy的报道,且具有良好的充放电循环特性和柔韧性,有望在便携式电子器件上得到应用。
3、NPG/金属氧化物薄膜复合材料及其电化学电容性能的研究
我们通过一种简单的电化学方法制备了纳米多孔金(NPG)/过渡金属氧化物(Cox、RuO2)复合材料,氧化物材料具有连续的层状结构并与NPG形成三明治夹心结构。该材料以NPG为结构支撑和集电器,而过渡金属氧化物提供高的比电容,从而提高材料整体电容。实验结果表明,氧化钴的体积和质量比电容分别达到了598F cm-3和563Fg-1,并且该材料表现出优异的稳定性。
虽然许多结构材料可以得到高的质量比电容,但是它们的活性材料载量较低,限制了表观电容的提高。比起质量比电容许多应用领域如小尺寸电子产品或传统能量储存装置显然更在意表观电容量。本工作利用独立支撑的NPG电极作为衬底材料,制备NPG/RuO2复合材料,以期获得较大的表观电容。NPG可同时作为集流器和结构支撑材料,Ru02作为电容活性材料。实验结果表明Ru02的电容高达520Fg-1,NPG/RuO2复合材料的表观电容达到了1.5Fcm-2,并且具有优良的倍率性能和较好的稳定性。
4、MnOx纳米线/大孔金属复合材料及其电化学电容性能研究
超级电容器因具有高的功率密度、长循环寿命和良好的安全性能被广泛应用于混合电动车能源系统、数字远程通信系统、不间断电源、脉冲激光技术等领域。比起质量比电容许多应用领域更在意高的表观电容量。本工作通过水热合成的方法制备了MnOx纳米线/大孔金属复合材料,该材料使用泡沫镍的网状结构为氧化锰纳米线提供良好的导电性,开孔的三维结构可以提供畅通的电解液通道,为离子传输提供方便。相互缠绕堆积的氧化锰纳米线首先依靠相互之间的联系提供赝电容,继而通过三维网状结构基底完成充放电过程。实验结果表明,MnOx质量比电容为576Fg-1,而本实验所得泡沫镍/MnOx样品的表观电容值达到了7.6Fcm-2,且表现出较好的稳定性。
The extensive dependence on fossil fuels has caused significant environmental pollution as well as energy resource crisis. Sustainable exploration and use of energy source depend on discovery of new energy source and development of novel energy devices. As a kind of energy storage device, supercapacitors have many advantages over conventional batteries:high power density, long cycling stability, fast charge-discharge rate and being environment friendly. Wide research of nanoscale materials has promoted flourish of advanced energy storage technology. However, common problems involved with nanomaterials such as bad structural continuity, conglomeration and structural instability have restricted their application in supercapacitors. This work introduces strategies based on design of porous materials with high area aiming at improve the performance of the supercapacitors. We have conducted the design, synthesis and performance research of the electrode materials containing:the composite of porous metal materials with transition metal oxide and conducting polymers, one dimensional structural composite and macroporous metal/metal oxide hybrid materials. We demonstrate the above composite materials have wide prospect for application in the supercapacitors as well as other similar fields.
1. Controllable synthesis of MnO2/polyaniline nanocomposite and its electrochemical capacitive property.
Polyaniline (PANI) and MnO2/PANI composites are simply and controllably fabricated by one-step interfacial polymerization at various pH. The morphologies and components of MnO2/PANI composites are modulated by changing pH of the solution. Formation procedure and capacitive property of the products are investigated by XRD,FTIR, TEM and electrochemical techniques. We demonstrate that MnO2as an intermedia material plays a key role in the formation of sample structures. The MnO2/PANI composites exhibit good cycling stability as well as a high capacitance close to207F g-1. Samples fabricated with the facile one-step method are also expected to be adopted in other field such as catalysis, lithium ion battery and biosensor.
2. Sub-micrometer-thick all-solid-state supercapacitors with high power and energy densities.
Fast development of portable and miniature electrics desires compatible energy conversion and storage devices. A flexible NPG-PPy composite film was fabricated using a convenient dealloying and electro-polymerization process. The bicontinuous pore/ligament structure provides high electric conductivity as well as improved ionic transferring channels, which increases the efficiency of the active materials. All-solid-state supercapacitors were designed with NPG-PPy films as both electrodes and PVA as both the separator and electrolyte. The symmetric supercapacitor thus-produced offers large specific capacitance, power density and energy density (296kW kg-1and27Wh kg-1), and exhibits almost identical performance at various curvatures, which suggests its wide application prospect in powering wearable/miniaturized electronics.
3. Electrochemical capacitive behavior of metal oxide and nanoporous gold hybrid structure.
Cobalt oxide and nanoporous gold (NPG) hybrid films are fabricated by a facile electrochemical technique. Structural morphology, composition and capacitive behavior of the sample have been investigated. The composite film has a sandwich like structure containing NPG film as the inside layer and cobalt oxide films as outside layers. NPG, as a3dimensional interconnected skeleton, can afford electron and ion transfer channels thus improve the efficiency of cobalt oxide. The hybrid films provide high volumetric (598F cm-3) and gravimetric capacitances (563F g-1), additionally exhibit good stibility.
To improve the apparent capacitance of the supercapacitors, we chose the ideal capacitive material RuO2as the active electrode material. NPG/RuO2composites are synthesized by CV method using NPG as the substrate and the corrent collectors. The gravimetric capacitance of RuO2achieves502F g-1, and the volumetric capacitance of the composite is close to1.5F g-1.
4. MnOx Nanowires aligned on the macroporous structures with high volumetric electrochemical capacitance.
Because of their high power densities, long lifespan and safe operation, supercapacitors have been used in the areas of hybrid vehicles, digital telecommunication systems, uninterrupted backup energy systems and pulsed laser techniques. The fast development of electronic techniques such as portable electronics or stationary energy storage devices poses new challenges for the design and fabrication of compatible energy devices with large amount of energy stored per area as well as energy per mass. For this work, we propose a facile hydrothermal synthesis method for MnOx nanowires aligned on Ni foam. As prepared porous nanostructures can provide fast electronic transferring channels and reduce ionic diffusion distance with enlarged electrode/electrolyte contact area. The entangled MnOx nanowires provide high pseudocapacitance, and the porous Ni foam serves as substrate and current collectors. The capacitance per mass and area are estimated as high as576F g-1and7.6F cm-2.
引文
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