【摘要】：隨著全球能源消耗的日益增長和環(huán)境的迅速惡化,開發(fā)清潔新能源受到各國科學家的廣泛關(guān)注。超級電容器作為一種新型儲能裝置,具有功率密度高、充放電速度快、循環(huán)壽命長和對環(huán)境友好等優(yōu)點,被廣泛應用于各大領(lǐng)域。隨著便攜式電子產(chǎn)品的柔性化和輕薄化,開發(fā)柔性全固態(tài)超級電容器就成了研究熱點。超級電容器性能的好壞取決于電極材料的選取,過渡金屬硫化物因其理論容量高,導電性好等優(yōu)點,得到廣泛應用。碳納米管(CNT)具有很好的柔韌性和機械穩(wěn)定性,通常被當作支架來構(gòu)筑混雜結(jié)構(gòu)。因此,把CNT與過渡金屬硫化物有效的結(jié)合起來,既提高器件的柔韌性,又提高了比容量。本論文以硫化銅(CuS)、硫化鋅(ZnS)和硫化錳(MnS)與CNT為核心,采用簡單的水熱合成法成功制備了形貌各異的復合納米材料,并將其應用在柔性全固態(tài)超級電容器中,展現(xiàn)出優(yōu)異的電化學性能。本論文主要研究成果如下:(1)通過工藝簡單的兩步水熱合成法在CNT外圍均勻生長一層CuS納米針,把合成的CuS@CNT復合納米材料用于超級電容器中,在1 A g-1的電流密度下,比電容高達566.4 F g-1。進一步把硫與CuS@CNT復合,合成S@CuS@CNT復合材料用于鋰硫電池中。當電流密度為0.1 C時,電池容量達到1019 mA h g-1。(2)通過基于模板的簡單水熱法在CNT外圍成功合成了一層超薄ZnS納米片,構(gòu)成ZnS@CNT復合材料。通過改變Zn(NO3)2的濃度和水熱反應時間,展示了超薄ZnS納米片的形成過程。又通過與單純的ZnS納米球?qū)Ρ?ZnS@CNT擁有更大的比表面積,有利于離子在電解液中擴散,因而展示出了更好的電化學性能。將此電極材料組裝成對稱全固態(tài)超級電容器,在1 A g-1測試下比電容達到159.6 F g-1,最后把四個器件串聯(lián)起來,對其充電,能點亮不同顏色的發(fā)光二極管。(3)通過低成本的水熱反應成功在CNT外圍均勻的生長一層γ-MnS納米顆粒。先在CNT周圍生長一層二氧化硅(Si O2),有利于γ-MnS沿CNT縱軸垂直生長,最后加入硫化鈉(Na2S),既提供硫源同時又能去除Si O2。改變水熱反應時間,實現(xiàn)了γ-MnS@CNT形貌各異的可控合成。將材料用于超級電容器中,在0.5 A g-1測試下比電容高達641.9 F g-1,對其進行3000圈充放電后,容量保持率高達94.6%。最后組裝成對稱柔性全固態(tài)超級電容器,也展現(xiàn)出了優(yōu)異的電化學性能。
[Abstract]:With the increasing global energy consumption and the rapid deterioration of the environment, the development of clean new energy has been widely concerned by scientists all over the world. As a new type of energy storage device, supercapacitor is widely used in many fields because of its high power density, high charge and discharge speed, long cycle life and environmental friendliness. With the flexibility and thinning of portable electronic products, the development of flexible all-solid-state supercapacitors has become a research hotspot. The performance of supercapacitors depends on the selection of electrode materials. Transition metal sulfides are widely used because of their high theoretical capacity and good conductivity. Carbon nanotubes (CNT) have good flexibility and mechanical stability and are often used as scaffolds to construct hybrid structures. Therefore, the combination of CNT and transition metal sulfides can not only improve the flexibility of the devices, but also improve the specific capacity. In this thesis, copper (CuS), zinc sulfide (ZnS) and manganese sulfide (MnS) and CNT (manganese sulfide) were used as core materials to prepare composite nanomaterials with different morphologies by hydrothermal synthesis method, and they were used in flexible all-solid supercapacitors. Show excellent electrochemical performance. The main research results of this thesis are as follows: (1) A layer of CuS nanowires was uniformly grown on the periphery of CNT by a simple two-step hydrothermal synthesis method. The synthesized CuS@CNT nanocomposites were used in supercapacitors at the current density of 1 Ag ~ (-1). The specific capacitance is up to 566.4 F g -1. Furthermore, S@CuS@CNT composite was synthesized by combining sulfur with CuS@CNT and used in lithium sulfur battery. When the current density is 0. 1 C, the capacity of the cell reaches 1019 mA h g -1. (2) an ultrathin ZnS nanocrystalline was synthesized on the periphery of CNT by a simple hydrothermal method based on template. By changing the concentration of Zn (NO3) 2 and hydrothermal reaction time, the formation process of ultrathin ZnS nanoparticles was demonstrated. Compared with the pure ZnS nanospheres, it has a larger specific surface area, which is conducive to the diffusion of ions in the electrolyte, thus showing a better electrochemical performance. The electrode material was assembled into a symmetrical all-solid supercapacitor, and the specific capacitance reached 159.6 F g-1 under 1 A g ~ (-1) test. Finally, the four devices were connected in series and charged. Light emitting diodes of different colors can be illuminated. (3) A layer of 緯 -MnS nanoparticles was successfully grown on the periphery of CNT by low cost hydrothermal reaction. A layer of silicon dioxide (Si O 2) was grown around CNT, which was beneficial to the vertical growth of 緯 -MnS along the longitudinal axis of CNT. Finally, the addition of sodium sulfide (Na2S) provided both sulfur source and Si O 2 removal. The controllable synthesis of 緯 -MnSCNT with different morphologies was achieved by changing the hydrothermal reaction time. When the material is used in supercapacitor, the specific capacitance is up to 641.9 F g ~ (-1) under 0.5 A g ~ (-1) test. After 3000 cycles of charge and discharge, the capacity retention rate is as high as 94.6%. Finally, symmetrical flexible all-solid state supercapacitors were assembled and showed excellent electrochemical performance.
【學位授予單位】：信陽師范學院
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TB383.1;TM53

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