本文選題：直接甲醇燃料電池 + 功能化石墨烯��； 參考：《新疆大學(xué)》2015年碩士論文

【摘要】：直接甲醇燃料電池(DMFC)具有結(jié)構(gòu)簡(jiǎn)單和能量轉(zhuǎn)化效率高等特點(diǎn),被認(rèn)為是一種新型綠色的環(huán)保能源,越來(lái)越受到人們的關(guān)注。催化劑的活性和穩(wěn)定性是影響DMFC商業(yè)化的重要因素之一。因此,制備具有較高催化活性和穩(wěn)定性的催化劑成為DMFC的研究熱點(diǎn),其中載體對(duì)催化劑的性能起著關(guān)鍵性的作用;石墨烯具有良好的物理和化學(xué)性能,在催化劑載體方面有潛在的應(yīng)用前景。本文以功能化石墨烯為載體負(fù)載Pt,制備了直接甲醇燃料電池陽(yáng)極催化劑,并研究了電催化活性及穩(wěn)定性。主要研究結(jié)果如下:1.采用高溫?zé)峤饩郾桨沸揎椀难趸?PANI-GO),通過(guò)改變氧化石墨烯與苯胺(GO/ANI)的質(zhì)量比,制備了一系列氮摻雜還原氧化石墨烯碳材料(N-RGO),以其負(fù)載Pt合成了Pt/N-RGO納米結(jié)構(gòu)電催化劑。采用透射電鏡(TEM)、X射線衍射譜(XRD)、拉曼光譜(Raman)及X射線光電子能譜(XPS)等技術(shù)對(duì)Pt/N-RGO的形貌及結(jié)構(gòu)進(jìn)行表征。用循環(huán)伏安和計(jì)時(shí)電流等電化學(xué)技術(shù)研究了Pt/N-RGO電極催化劑對(duì)CO溶出反應(yīng)和甲醇電氧化反應(yīng)的催化性能。發(fā)現(xiàn)GO/ANI質(zhì)量比為1:1.3時(shí)所制備Pt/N-RGO(1:1.3)催化劑顯示出最好的抗CO中毒能力;催化甲醇氧化的電流密度達(dá)到160.8 A·g-1;與未摻雜氮樣品Pt/RGO相比,Pt/N-RGO(1:1.3)樣品顯示出更強(qiáng)的抗CO中毒能力和更高的甲醇電氧化催化活性及穩(wěn)定性。2.以苯胺(ANI)及聚苯胺(PANI)對(duì)還原氧化石墨烯(RGO)進(jìn)行非共價(jià)修飾,并以其為載體負(fù)載Pt制備了Pt/ANI-RGO和Pt/PANI-RGO催化劑。結(jié)果顯示,ANI及PANI對(duì)RGO進(jìn)行修飾能明顯減小Pt納米顆粒的尺寸和分布范圍;ANI及PANI的引入,提高了催化劑Pt的電化學(xué)活性面積,所制備的Pt/ANI-RGO和Pt/PANI-RGO催化劑對(duì)甲醇氧化的催化活性(125.6 A·g-1和86.4 A·g-1)要高于Pt/RGO催化劑(77.3 A·g-1),但ANI及PANI對(duì)RGO的修飾對(duì)RGO負(fù)載的Pt電催化劑的催化穩(wěn)定性沒(méi)有影響。3.采用聚乙烯吡咯烷酮(PVP)非共價(jià)修飾的RGO為載體,以其負(fù)載Pt得到Pt/PVP-RGO催化劑。結(jié)果顯示,Pt/PVP-RGO催化劑表面的Pt顆粒分布均勻、尺寸較小;相對(duì)于Pt/RGO催化劑而言,PVP的加入,對(duì)Pt/PVP-RGO催化劑甲醇氧化活性無(wú)顯著改善;但Pt/PVP-RGO催化劑的穩(wěn)定性(下降51%)明顯高于Pt/RGO催化劑(下降62%),PVP的存在對(duì)催化劑穩(wěn)定性的提高有一定的積極作用。4.利用甲基紫精(MV)非共價(jià)功能化RGO,并以其負(fù)載Pt制備了Pt/MV-RGO納米催化劑。結(jié)果表明,Pt/MV-RGO催化劑表面的Pt顆粒分布狀況和尺寸大小有明顯改善;Pt/MV-RGO催化劑的電化學(xué)活性面積為24.7 m2·g-1,是Pt/RGO的3倍;同時(shí),Pt/MV-RGO催化劑催化甲醇氧化的電流密度為221.4 A·g-1,是Pt/RGO的2.6倍;在氧還原反應(yīng)中Pt/MV-RGO催化劑亦有著較高的催化活性,Pt/MV-RGO催化劑的穩(wěn)定性也較好。
[Abstract]:Direct methanol fuel cell (DMFC), which has the characteristics of simple structure and high energy conversion efficiency, is considered as a new type of green environmental energy, which has attracted more and more attention. The activity and stability of the catalyst is one of the important factors affecting the commercialization of DMFC. Therefore, the preparation of catalysts with high catalytic activity and stability has become a research hotspot in DMFC, in which the support plays a key role in the performance of the catalyst, and graphene has good physical and chemical properties. It has potential application prospect in catalyst support. In this paper, the anode catalyst for direct methanol fuel cell was prepared with functionalized graphene as the carrier, and its electrocatalytic activity and stability were studied. The main results are as follows: 1. A series of nitrogen-doped reduced graphene oxide carbon materials (N-RGON) were prepared by changing the mass ratio of graphene oxide to aniline in the presence of high temperature Polyaniline modified graphene oxide (PANI-GON). A series of nitrogen-doped graphene oxide carbon materials (N-RGON) were prepared by supported Pt to synthesize Pt/N-RGO nanostructure electrocatalysts. The morphology and structure of Pt/N-RGO were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), Raman spectroscopy (Raman) and X-ray photoelectron spectroscopy (XPS). The catalytic properties of Pt/N-RGO electrode catalysts for CO dissolution and methanol electrooxidation were studied by cyclic voltammetry and chronoamperometry. When the mass ratio of GO/ANI is 1: 1.3, the catalyst prepared by Pt- / N-RGO1: 1.3) shows the best ability to resist CO poisoning. The current density of catalytic methanol oxidation reached 160.8 Ag-1.The Pt- / N-RGO1: 1.3) samples showed stronger resistance to CO poisoning and higher catalytic activity and stability of methanol electrooxidation than unadulterated nitrogen samples (Pt/RGO / RGO1: 1.3). Pt/ANI-RGO and Pt/PANI-RGO catalysts were prepared by noncovalent modification with aniline (ANI) and Polyaniline (Polyaniline), and supported on Pt. The results show that the modification of RGO by RGO and PANI can obviously reduce the size and distribution of Pt nanoparticles and increase the electrochemical active area of Pt. The catalytic activity of the prepared Pt/ANI-RGO and Pt/PANI-RGO catalysts for methanol oxidation was 125.6 Ag-1 and 86.4 Ag-1), which was higher than that of Pt/RGO catalyst 77.3 Ag-1G ~ (-1), but the modification of RGO by ANI and PANI had no effect on the catalytic stability of RGO supported Pt electrocatalyst. The non-covalent modified polyvinylpyrrolidone (PVP) RGO was used as the support and supported on Pt to obtain the Pt/PVP-RGO catalyst. The results showed that the Pt particles on the surface of PtP / PVP-RGO catalyst were uniformly distributed and the size of Pt particles was smaller than that of Pt/RGO catalyst, and the methanol oxidation activity of Pt/PVP-RGO catalyst was not significantly improved compared with the addition of PtPVP-RGO catalyst. However, the stability of Pt/PVP-RGO catalyst was significantly higher than that of Pt/RGO catalyst. Pt/MV-RGO nanocatalysts were prepared by non-covalent functionalization of methyl violet spermatine (MV) and supported on Pt. The results show that the distribution and size of Pt particles on the surface of Pt- / MV-RGO catalyst are obviously improved, the electrochemical activity area of Pt- MV-RGO catalyst is 24.7 m2 g ~ (-1), which is 3 times of that of Pt/RGO, and the current density of methanol oxidation is 221.4 Ag-1, 2.6 times of that of Pt/RGO, while the current density of Pt- / MV-RGO catalyst is 221.4 Ag-1. In the oxygen reduction reaction, Pt/MV-RGO catalyst also has higher catalytic activity. The stability of Pt- MV-RGO catalyst is better than that of Pt- MV-RGO catalyst.
【學(xué)位授予單位】：新疆大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O643.36;TM911.4

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相關(guān)期刊論文 前1條

1 宋樹(shù)芹,梁振興,周衛(wèi)江,孫公權(quán),辛勤;DMFC的阻甲醇滲透研究進(jìn)展[J];電池;2004年04期

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本文編號(hào)：1876515