本文選題：CeO_2-CuO + 多孔材料��； 參考：《內(nèi)蒙古大學(xué)》2015年碩士論文

【摘要】：近年來(lái),化石能源的大量消耗導(dǎo)致的溫室效應(yīng)和資源枯竭等問(wèn)題日益突出。氫能作為一種安全可再生、無(wú)污染的新型能源,受到廣泛關(guān)注。其中,質(zhì)子交換膜燃料電池是較為有效的氫能利用方式。然而,目前所用的氫燃料中常含有0.3-1%的CO,會(huì)毒化燃料電池的Pt電極,縮短電池使用壽命。采用CO優(yōu)先氧化去除所含氫燃料中微量CO是最為有效的氫燃料凈化途徑之一。而貴金屬和非貴金屬催化劑是可應(yīng)用于富氫氣氛中CO優(yōu)先氧化的兩類(lèi)主要的催化劑。CeO2-CuO基催化劑作為非貴金屬催化劑的代表逐漸成為研究熱點(diǎn)。CeO2-CuO基非貴金屬催化劑原料來(lái)源廣泛,價(jià)格便宜,對(duì)CO有較高轉(zhuǎn)化率,對(duì)CO2有較好選擇性,在較高溫度有較好催化活性。然而,這類(lèi)催化劑反應(yīng)溫度窗口較窄,限制了其實(shí)際應(yīng)用。針對(duì)上述CeO2-CuO基催化劑的應(yīng)用瓶頸問(wèn)題,本文采用膠體晶體模板法,結(jié)合前驅(qū)體熱分解方法,制備了一系列多孔CeO2-CuO基催化材料,對(duì)其富氫氣氛中CO優(yōu)先氧化性能進(jìn)行了系統(tǒng)研究,獲得了在較寬溫度窗口具有優(yōu)異催化性能的CeO2-CuO基催化材料,該類(lèi)催化材料在質(zhì)子燃料膜電池氫燃料凈化領(lǐng)域具有重要的應(yīng)用價(jià)值。本文第一章對(duì)氫能與質(zhì)子燃料膜電池進(jìn)行了概述,并對(duì)富氫氣氛中CO優(yōu)先氧化催化材料的研究現(xiàn)狀進(jìn)行了綜述。本文第二章以膠體晶體為模板,利用前驅(qū)體熱分解方法制備了一系列多孔CeO2-CuO基催化材料。所制備的CeO2-CuO基催化材料具有連貫有序的大孔結(jié)構(gòu),孔徑約為200 nm。同時(shí),大孔結(jié)構(gòu)的孔壁存在3-4 nm的介孔,形成大孔-介孔共存的多孔結(jié)構(gòu)。這類(lèi)大孔-介孔結(jié)構(gòu)共存的多孔結(jié)構(gòu)的形成,導(dǎo)致CeO2-CuO基催化材料具有較大的比表面積,Ce02與CuO之間產(chǎn)生強(qiáng)的協(xié)同相互作用,使其在富氫氣氛中具有優(yōu)異的CO優(yōu)先氧化性能。同時(shí),通過(guò)在CeO2-CuO基催化材料中引入CO304和Fe203等助催化劑,可在一定程度上調(diào)節(jié)CO優(yōu)先氧化反應(yīng)的溫度窗口,使其在較寬的反應(yīng)溫度窗口展現(xiàn)出優(yōu)異的CO優(yōu)先氧化性能。本文第三章以膠體晶體為模板,利用前驅(qū)體熱分解方法制備了多孔Ce02,并采用沉積-沉淀法在Ce02上負(fù)載了CuO,制備了多孔CuO/CeO2基催化材料。所制備的多孔CuO/CeO2基催化材料孔徑均一,連貫有序,比表面積較大。CuO/CeO2基催化材料在富氫氣氛中CO優(yōu)先氧化的反應(yīng)活性測(cè)試顯示,CO選擇性隨著CuO負(fù)載量的增加而升高,當(dāng)CuO負(fù)載量達(dá)到10%時(shí),對(duì)CO選擇性達(dá)到最佳。此時(shí),CuO多以高分散狀態(tài)分布于Ce02表面,高分散的CuO物種與Ce02間的強(qiáng)的相互協(xié)同作用,極大地促進(jìn)了富氫氣氛中CO優(yōu)先氧化反應(yīng)的進(jìn)行。本文第四章對(duì)論文研究工作進(jìn)行了總結(jié),并對(duì)未來(lái)研究進(jìn)行了展望。
[Abstract]:In recent years, the problems of Greenhouse Effect and resource depletion caused by fossil energy consumption have become increasingly prominent.Hydrogen energy, as a kind of safe renewable, non-polluting new energy, has received extensive attention.Among them, proton exchange membrane fuel cell (PEMFC) is an effective way to utilize hydrogen energy.However, the hydrogen fuel used at present often contains 0.3-1% of CO. it can poison Pt electrode of fuel cell and shorten the life of fuel cell.The removal of trace CO from hydrogen fuel by CO preferential oxidation is one of the most effective ways to purify hydrogen fuel.However, noble metal and non-noble metal catalysts are two main catalysts for CO preferential oxidation in hydrogen-rich atmosphere. CeO2-CuO-based catalysts, as representatives of non-noble metal catalysts, have gradually become the focus of research. CeO2-CuO based non-noble metal catalysts have been widely used as raw materials.It has the advantages of lower price, higher conversion of CO, better selectivity to CO2, and better catalytic activity at higher temperature.However, the temperature window of this kind of catalyst is narrow, which limits its practical application.In this paper, a series of porous CeO2-CuO catalyst materials were prepared by colloidal crystal template method and precursor thermal decomposition method. The catalytic properties of CO preferential oxidation in hydrogen-rich atmosphere were systematically studied.CeO2-CuO based catalytic materials with excellent catalytic performance in a wide temperature window have been obtained, which have important application value in hydrogen fuel purification of proton fuel membrane cells (PEMFC).In the first chapter, hydrogen energy and proton fuel membrane cells are reviewed, and the research status of catalytic materials for CO preferential oxidation in hydrogen-rich atmosphere is reviewed.In the second chapter, a series of porous CeO2-CuO based catalytic materials were prepared by thermal decomposition of precursor using colloidal crystal as template.The prepared CeO2-CuO-based catalyst has a coherent and ordered macroporous structure with a pore size of about 200 nm.At the same time, there are 3-4 nm mesopore in the pore wall of the macroporous structure, forming a porous structure with macroporous and mesoporous coexistence.The formation of this kind of porous structure with macroporous and mesoporous structure leads to a strong synergistic interaction between Ce02 and CuO with large specific surface area, which results in excellent CO preferential oxidation performance in hydrogen-rich atmosphere.At the same time, the temperature window of CO preferential oxidation reaction can be adjusted to a certain extent by introducing CO304 and Fe203 cocatalysts into CeO2-CuO based catalytic materials, so that the excellent CO preferential oxidation performance can be shown in the wider reaction temperature window.In the third chapter, porous ce _ (02) was prepared by thermal decomposition of precursor using colloidal crystal as template, and CuO was supported on Ce02 by deposit-precipitation method to prepare porous CuO/CeO2 based catalytic material.The pore size uniformity, coherence and order of the porous CuO/CeO2 catalyst materials, and the large specific surface area of CuO / CEO _ 2 based catalyst materials, showed that the CO selectivity increased with the increase of the amount of CuO loading in the hydrogen-rich atmosphere.When the load of CuO reaches 10, the selectivity of CO is optimized.In this case, the highly dispersed CuO species are distributed on the surface of Ce02, and the strong interaction between highly dispersed CuO species and Ce02 greatly promotes the CO preferential oxidation in hydrogen-rich atmosphere.The fourth chapter summarizes the research work and prospects for future research.
【學(xué)位授予單位】：內(nèi)蒙古大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類(lèi)號(hào)】：O643.36;TM911.4

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本文編號(hào)：1760898