本文關(guān)鍵詞：石墨烯片層和氮摻雜碳納米籠的制備及其應(yīng)用研究　出處：《華東理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 石墨烯 碳納米籠 催化活性 耐久性 N摻雜

【摘要】：石墨烯片層(Graphene Nano Sheets, GNS)和碳納米籠(Carbon Nano Cages, CNCs)是兩類非常重要的碳納米材料。GNS在納米電子器件,太陽(yáng)能電池,燃料電池催化劑等多領(lǐng)域有重要的應(yīng)用價(jià)值,CNCs由于其獨(dú)特的中空結(jié)構(gòu),較高的石墨化程度在存儲(chǔ),電子器件,燃料電池,藥物載體等方面有潛在的應(yīng)用前景。目前如何大量制備高質(zhì)量GNS是亟待解決的問(wèn)題。在燃料電池應(yīng)用方面,GNS作為載體有望提升Pt催化劑耐久性。燃料電池催化劑仍然面臨Pt催化劑成本過(guò)高的問(wèn)題,研究表明,N摻雜碳材料具有一定的氧還原催化活性(ORR),如何制備高N含量高比表面積碳納米材料也是研究的熱點(diǎn)之一。針對(duì)上述兩個(gè)問(wèn)題,本論文分別在GNS的連續(xù)化制備和高N含量CNCs制備以及它們?cè)谌剂想姵貞?yīng)用等方面進(jìn)行了重點(diǎn)研究。首先本文采用噴射裂解法,以羰基鐵為催化劑前驅(qū)體,吡啶為碳源,通過(guò)調(diào)節(jié)鐵/碳比和反應(yīng)溫度,實(shí)現(xiàn)了GNS連續(xù)化制備,并將其用作Pt催化劑載體,研究催化劑耐久性。為了制備高N含量高比表面積CNCs,本文采用浮動(dòng)氣相沉積法,以液態(tài)羰基鐵為催化劑前驅(qū)體,乙炔為碳源,氨氣為氮源,制備實(shí)心CNC,利用NH4Cl除鐵,再經(jīng)氨氣熱處理,得到N摻雜空心CNCs,并將其作為ORR催化劑,考察其催化活性和耐久性。本文制備的GNS層數(shù)約為3-5層,具有良好的石墨化結(jié)構(gòu)(IG/ID=2.8)和一定的N含量(3.42 at.%)。作為催化劑載體時(shí),通過(guò)液相還原法在其表面均勻沉積納米Pt顆粒,得到Pt/GNS催化劑,催化劑展現(xiàn)了高催化活性和優(yōu)秀的耐久性。實(shí)驗(yàn)制備N摻雜CNCs具有非常高的比表面積(1344 m2 g-1),高N含量(5.3 at.%)。在酸性介質(zhì)中,作為ORR催化劑展現(xiàn)出與商業(yè)Pt/C相當(dāng)?shù)碾姶呋钚院透鼉?yōu)異的耐久性�；谶@些研究有望促進(jìn)GNS的連續(xù)化制備研究和商業(yè)化應(yīng)用。N摻雜CNCs作為一種重要的無(wú)貴金屬催化劑將會(huì)在燃料電池領(lǐng)域有很好的應(yīng)用前景。
[Abstract]:Graphene Nano sheets and carbon Nano Cages. CNCsare two kinds of very important carbon nano-materials. GNS has important application value in many fields such as nano-electronic devices solar cells fuel cell catalysts and so on. Due to its unique hollow structure, CNCs has a higher degree of graphitization in storage, electronic devices, and fuel cells. Drug carriers and other potential applications. How to prepare a large number of high-quality GNS is an urgent problem. In fuel cell applications. GNS is expected to improve the durability of Pt catalyst. The fuel cell catalyst still faces the problem of high cost of Pt catalyst. N-doped carbon materials have a certain catalytic activity of oxygen reduction. How to prepare high N content and high specific surface area carbon nanomaterials is one of the hot topics. In this thesis, the continuous preparation of GNS, the preparation of high N content CNCs and their applications in fuel cells were studied. Firstly, jet pyrolysis method was used in this paper. Using iron carbonyl as catalyst precursor and pyridine as carbon source, continuous preparation of GNS was realized by adjusting iron / carbon ratio and reaction temperature, and used as Pt catalyst support. In order to prepare CNCswith high N content and high specific surface area, liquid carbonyl iron was used as catalyst precursor, acetylene as carbon source and ammonia as nitrogen source in order to prepare CNCswith high N content and high specific surface area. Solid CNCs were prepared by using NH4Cl to remove iron and then treated with ammonia gas to obtain N-doped hollow CNCs and used as ORR catalysts. The catalytic activity and durability were investigated. The number of GNS layers prepared in this paper is about 3-5 layers. It has a good graphitization structure and a certain N content of 3.42 at.0.When it is used as catalyst support. Pt/GNS catalyst was obtained by homogeneous deposition of Pt nanoparticles on the surface by liquid phase reduction method. The catalyst exhibits high catalytic activity and excellent durability. The experimental preparation of N-doped CNCs has a very high specific surface area of 1344m2 / g ~ (-1). The high N content is 5.3 at.0.It is in acid medium. As a ORR catalyst, the electrocatalytic activity is comparable to that of commercial Pt/C with better durability. Based on these studies, it is expected to promote the continuous preparation of GNS and the commercial application of .N-doped CNCs. As an important noble metal-free catalyst, it will have a good prospect in the field of fuel cells.
【學(xué)位授予單位】：華東理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TQ127.11;TB383.1

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本文編號(hào)：1407908