本文關(guān)鍵詞： 瀝青質(zhì) 預(yù)氧化 氮摻雜 物理活化 超級(jí)電容器　出處：《大連理工大學(xué)》2015年碩士論文　論文類(lèi)型：學(xué)位論文

【摘要】：氮摻雜多孔炭材料由于具有獨(dú)特機(jī)械、光學(xué)、電子等特性使得其在儲(chǔ)能、催化、分離等領(lǐng)域中顯示出誘人的應(yīng)用前景。研究熱處理制備過(guò)程中摻氮炭材料的結(jié)構(gòu)、組成及表面化學(xué)性質(zhì)的變化特點(diǎn),對(duì)于實(shí)現(xiàn)炭材料定向摻氮具有重要意義。本文主要以煤液化殘?jiān)鶠r青質(zhì)為碳源,MS為氮源,制備氮摻雜炭材料,主要研究成炭熱處理過(guò)程中氮摻雜炭材料表面官能團(tuán)的變化；在此基礎(chǔ)上通過(guò)CO2活化法制備了氮摻雜的多孔炭材料,并測(cè)試了摻氮多孔炭材料的電化學(xué)性能。主要研究?jī)?nèi)容和成果如下：(1)熱處理過(guò)程中氮摻雜炭材料表面官能團(tuán)的變化研究瀝青質(zhì)(A)經(jīng)預(yù)氧化得到預(yù)氧化的瀝青質(zhì)(AO),將預(yù)氧化后的瀝青質(zhì)(AO)與氮源(MS)混合放入管式爐中,在不同溫度、氮?dú)猸h(huán)境下進(jìn)行熱處理制備氮摻雜炭材料(AOM-Ts),主要研究熱處理溫度變化過(guò)程中氮摻雜炭材料表面官能團(tuán)的演變規(guī)律。結(jié)果表明：相比于A(yíng),AO在熱處理過(guò)程中表現(xiàn)出較好的熱穩(wěn)定性,在熱處理溫度為800℃時(shí)其炭化收率高達(dá)63.75%；經(jīng)處理的AO出現(xiàn)了明顯的羰基官能團(tuán),所含氧元素含量明顯高于A(yíng),這些含氧官能團(tuán)的存在為MS中的-NH2反應(yīng)提供了豐富的活性位；熱處理溫度在500℃以上時(shí),在相同的熱處理溫度下,AOM-T的氮元素、氧元素的含量高于A(yíng)M-T；對(duì)于樣品AOM-Ts而言,熱處理溫度在500℃之前,含氮官能團(tuán)主要以N-5和N-6兩種形式存在；熱處理溫度為600℃時(shí),含氮官能團(tuán)出現(xiàn)了N-Q,700℃時(shí)出現(xiàn)了N-X；隨著熱處理溫度的升高,N-5的含量基本上保持不變,N-6的含量逐漸降低,而N-X和N-Q的含量均增加；熱處理溫度的變化對(duì)含氧官能團(tuán)存在的形態(tài)沒(méi)有明顯的影響,均以O(shè)-Ⅰ和O-Ⅱ類(lèi)型存在,且O-Ⅱ的含量大于O-Ⅰ的含量。(2)瀝青質(zhì)氧化前后對(duì)摻氮炭材料表面組成、結(jié)構(gòu)以及電化學(xué)性能的影響分別以瀝青質(zhì)/預(yù)氧化的煤液化殘?jiān)鼮r青質(zhì)為原料、MS為氮源,采用CO2物理活法制備氮摻雜的多孔炭材料,研究瀝青質(zhì)預(yù)氧化處理工藝對(duì)其摻氮造孔后的組成、結(jié)構(gòu)以及電化學(xué)性能的影響。結(jié)果表明：預(yù)氧化后的樣品中所含的氮元素含量、N-5和N-6總含量、比表面積和孔容均明顯變大,其含氮量為4.85 wt.%,比表高達(dá)986 m2.g-1,孔容為0.61cm3.g-1；在三電極體系下,6 M KOH電解液中100 mA·g-1的電流密度下,預(yù)氧化處理后的樣品具有最大的質(zhì)量比電容,其值為197 F·g-1；當(dāng)電流密度達(dá)到10 A·g-1時(shí),其質(zhì)量比電容仍可達(dá)到136 F·g-1；在兩電極體系、1 A·g-1的電流密度下,經(jīng)過(guò)5000次循環(huán)充放電,其電容值的保持率在90%以上,表現(xiàn)出良好的充放電循環(huán)性能。
[Abstract]:Nitrogen doped porous carbon materials have shown attractive applications in the fields of energy storage, catalysis and separation due to their unique mechanical, optical and electronic properties. The change of composition and surface chemical properties is of great significance to realize the directional nitrogen doping of carbon materials. In this paper, nitrogen doped carbon materials are prepared by using coal liquefaction residue based asphaltene as carbon source and MS as nitrogen source. The changes of functional groups on the surface of nitrogen-doped carbon materials during heat treatment were studied, and the nitrogen-doped porous carbon materials were prepared by CO2 activation method. The electrochemical properties of nitrogen-doped porous carbon materials were tested. The main research contents and results are as follows: 1) the changes of functional groups on the surface of nitrogen doped carbon materials during heat treatment; The pre-oxidized asphaltene (AO) and nitrogen source (MSS) are mixed into a tube furnace. At different temperatures, Nitrogen doped carbon materials were prepared by heat treatment in nitrogen atmosphere. The evolution of surface functional groups of nitrogen doped carbon materials during heat treatment temperature change was studied. The results showed that compared with AAO, the surface functional groups of nitrogen doped carbon materials showed better thermal stability during heat treatment. The carbonization yield is up to 63.75 at the heat treatment temperature of 800 鈩，

本文編號(hào)：1535722