【摘要】：碳納米管海綿是一種由多壁碳納米管無序堆積而成的三維多孔網(wǎng)絡(luò)結(jié)構(gòu),在能源和環(huán)境領(lǐng)域有廣闊的應(yīng)用前景。為了推動(dòng)碳納米管海綿的實(shí)際應(yīng)用,需要進(jìn)一步改善它的力學(xué)和電學(xué)等相關(guān)性能,尤其是在形變過程中的結(jié)構(gòu)穩(wěn)定性和彈性回復(fù)能力。此外,在碳納米管海綿內(nèi)部可控的引入活性材料是制備高性能功能器件的有效途徑。本論文研究了基于碳納米管海綿的復(fù)合多孔材料的可控制備、力學(xué)性能和電容性能,探索了在能源器件領(lǐng)域的應(yīng)用。通過在海綿內(nèi)部均勻負(fù)載非晶碳和導(dǎo)電聚合物制備了結(jié)構(gòu)可控的復(fù)合多孔材料,分別提高了海綿的力學(xué)性能和電化學(xué)性能。具體結(jié)果如下:制備了碳納米管/非晶碳復(fù)合多孔材料并研究了力學(xué)性能。采用化學(xué)氣相沉積法,乙炔為碳源,在海綿內(nèi)部直接沉積非晶碳,獲得了非晶碳均勻包覆的碳納米管核殼結(jié)構(gòu)。通過調(diào)節(jié)反應(yīng)時(shí)間等參數(shù)調(diào)控了包覆層的厚度,并且碳納米管之間的搭接點(diǎn)被有效焊接,形成了具有穩(wěn)定三維框架的塊體結(jié)構(gòu)。力學(xué)測(cè)試表明,引入非晶碳使碳納米管海綿的壓縮彈性模量和壓縮強(qiáng)度分別提高了40和60倍,在10%到50%的壓縮應(yīng)變下可彈性回復(fù),循環(huán)壓縮1000次后不產(chǎn)生塑性變形。分析了有關(guān)機(jī)制,發(fā)現(xiàn)碳納米管的包覆及焊接能夠保持材料在壓縮過程中的結(jié)構(gòu)穩(wěn)定性,從而獲得超彈性。制備了碳納米管/聚苯胺復(fù)合多孔材料并研究了電化學(xué)性能。采用電化學(xué)沉積法,苯胺單體為原料,在碳納米管海綿內(nèi)部聚合成聚苯胺,獲得了聚苯胺均勻包覆的碳納米管核殼結(jié)構(gòu),并且聚苯胺的厚度可調(diào),碳納米管之間的搭接點(diǎn)也被焊接。采用三電極法測(cè)試了復(fù)合海綿的電化學(xué)性能,發(fā)現(xiàn)引入聚苯胺使質(zhì)量比電容從約30 F/g提高到了753 F/g,高度壓縮后仍能保持70%以上的質(zhì)量比電容,同時(shí)體積比電容增加。通過在碳納米管和聚苯胺之間引入聚吡咯層,顯著提高了循環(huán)穩(wěn)定性(1000次循環(huán)后保持90%以上)。碳納米管的三維導(dǎo)電網(wǎng)絡(luò)以及表面均勻包覆的贗電容材料是提高電化學(xué)性能的兩個(gè)關(guān)鍵因素,在超級(jí)電容器領(lǐng)域有很好的應(yīng)用前景。
[Abstract]:Carbon nanotube sponge (CNT) is a three-dimensional porous network composed of multi-walled carbon nanotubes (MCNTs), which is widely used in the field of energy and environment. In order to promote the practical application of carbon nanotube sponge, it is necessary to further improve its mechanical and electrical properties, especially its structural stability and elastic recovery ability during deformation. In addition, the controllable introduction of active materials into the carbon nanotube sponge is an effective way to fabricate high-performance functional devices. In this paper, the controllable preparation, mechanical properties and capacitive properties of composite porous materials based on carbon nanotube sponges are studied, and the applications in the field of energy devices are explored. Composite porous materials with controllable structure were prepared by uniformly loading amorphous carbon and conducting polymer in the sponge. The mechanical and electrochemical properties of the sponge were improved respectively. The results are as follows: carbon nanotube / amorphous carbon composite porous materials were prepared and their mechanical properties were studied. Amorphous carbon was deposited directly in the sponge by chemical vapor deposition with acetylene as the carbon source. The core-shell structure of carbon nanotubes coated uniformly with amorphous carbon was obtained. The thickness of the coating layer was adjusted by adjusting the reaction time and the lap joint between the carbon nanotubes was welded effectively to form a block structure with a stable three-dimensional frame. Mechanical tests show that the compressive elastic modulus and compressive strength of carbon nanotube sponges are increased by 40 and 60 times respectively with the introduction of amorphous carbon. Elastic recovery can be achieved at compression strain of 10% to 50%, and no plastic deformation is produced after 1000 cycles compression. The mechanism is analyzed and it is found that the coating and welding of carbon nanotubes can keep the structural stability of the material during compression process and obtain superelasticity. Carbon nanotubes / Polyaniline composite porous materials were prepared and electrochemical properties were studied. Polyaniline was polymerized into Polyaniline in carbon nanotube sponge by electrochemical deposition with aniline monomer as raw material. The core-shell structure of carbon nanotube coated with Polyaniline was obtained, and the thickness of Polyaniline was adjustable. Lap joints between carbon nanotubes are also welded. The electrochemical performance of composite sponge was measured by three-electrode method. It was found that the specific capacitance of composite sponge was increased from about 30 F / g to 753 F / g with the addition of Polyaniline, and the mass specific capacitance was still over 70% and the volume specific capacitance was increased after high compression. By introducing polypyrrole layer between carbon nanotubes and Polyaniline, the cycle stability was improved significantly (over 90% after 1000 cycles). The three-dimensional conductive network of carbon nanotubes and the uniformly coated pseudo-capacitor materials are two key factors to improve the electrochemical performance of carbon nanotubes and have a good application prospect in the field of supercapacitors.
【學(xué)位授予單位】：哈爾濱工業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TB33

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