本文選題：電催化　切入點(diǎn)：脫合金化　出處：《太原理工大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：質(zhì)子交換膜燃料電池(PEMFC)是二十一世紀(jì)重要能源,新型能源燃料電池的特點(diǎn)包括比能量高、啟動迅速、環(huán)境友好、方便攜帶等,此類移動電源具有廣闊的發(fā)展前景。貴金屬顆粒是當(dāng)前燃料電池方面普遍使用的催化劑,以鉑,鈀貴金屬為主。而貴金屬具有價格昂貴、資源有限、易發(fā)生毒化等特點(diǎn),致使燃料電池的商業(yè)化發(fā)展較為遲緩。為了降低Pt、Pd的含量,提高其利用率,闡明催化劑貴金屬的含量和粒徑對催化劑的影響規(guī)律,進(jìn)一步提高其電催化性能,是值得深入研究的科學(xué)課題,也是解決目前Pt基催化劑大規(guī)模商業(yè)化發(fā)展的關(guān)鍵之一。本文通過改善負(fù)載物,載體和添加物方式研究其對催化劑的電催化活性影響,意義在于探索出高性能低成本的燃料電池陽極催化劑,為這一綠色新能源技術(shù)未來實(shí)現(xiàn)商業(yè)化提供更翔實(shí)的數(shù)據(jù)和理論依據(jù)。通過三種方式的調(diào)整合成貴金屬陽極催化劑,并探究其對有機(jī)小分子電催化性能的作用規(guī)律。主要研究分為以下三個部分:(1)通過液相還原法,制備Pd基催化劑,其中碳納米管為載體,控制Pd、Ag原子比為1:1(研究已表明,此種情況下催化性能最佳),通過添加不同含量的Cu元素,探討其催化劑性能提升的機(jī)理,研究系列Pd基催化劑在甲醇、乙醇和甲酸溶液中的電催化活性,結(jié)果表明Pd25Ag25Cu50/CNTs催化劑在甲醇、乙醇和甲酸氧化過程中展示出最佳的電催化活性,相比其它催化劑,穩(wěn)定性也達(dá)到最高。(2)引用新型載體,簡易Cu_3P-C復(fù)合載體策略來提高鉑納米顆粒對甲醇、乙醇、乙二醇和甲酸的電催化性能,控制Cu_3P與C的比例,探究發(fā)現(xiàn)當(dāng)Cu_3P與C的質(zhì)量比為1:1時,Pt/C-Cu_3P50%催化劑的電催化性能達(dá)到最高,說明復(fù)合載體的引入使Pt催化劑的催化活性得到提高。(3)引用添加物Fe_2P,探究Fe_2P不同比例含量下對Pt催化劑的電催化性能影響,其中Fe_2P含量較少且顆粒較小,區(qū)別于Cu_3P載體作用,分析其磷化物在較低含量下對甲酸、甲醇和乙醇的電催化活性影響。目前,磷化物作為新型材料,對燃料電池催化劑的電催化活性具有明顯的增強(qiáng)作用。結(jié)果發(fā)現(xiàn),添加物Fe_2P含量5%時達(dá)到合適的添加比例,此時Pt催化劑在甲醇,乙醇和甲酸有機(jī)小分子氧化過程中具有最佳的催化性能。
[Abstract]:Proton exchange membrane fuel cell (PEMFC) is an important energy source in 21th century. The characteristics of new energy fuel cell include high specific energy, quick start-up, friendly environment, easy to carry and so on. This kind of mobile power supply has broad development prospects. Precious metal particles are widely used catalysts in fuel cells at present, mainly platinum and palladium precious metals, while precious metals have the characteristics of high price, limited resources, easy to poison and so on. The commercial development of fuel cell is slow. In order to reduce the content of PtPd, improve the utilization rate, clarify the influence of the content and particle size of noble metal on the catalyst, and further improve its electrocatalytic performance. It is a scientific subject worthy of further study, and is also one of the keys to solve the large-scale commercial development of Pt-based catalysts. In this paper, the effects of Pt-based catalysts on their electrocatalytic activity are studied by improving the methods of support, support and additives. The significance lies in exploring the high performance and low cost anode catalyst for fuel cell, which will provide more detailed data and theoretical basis for the commercialization of this green new energy technology in the future. The PD based catalyst was prepared by liquid-phase reduction method, in which carbon nanotubes were used as the carrier, and the atomic ratio of PD / Ag was controlled to 1: 1. In this case, the best catalytic activity is obtained. The mechanism of improving the catalytic performance of the catalyst is discussed by adding different contents of Cu, and the electrocatalytic activity of a series of PD based catalysts in methanol, ethanol and formic acid solution is studied. The results showed that the Pd25Ag25Cu50/CNTs catalyst exhibited the best electrocatalytic activity in the oxidation of methanol, ethanol and formic acid, and the stability of the catalyst was the highest compared with other catalysts. The simple Cu_3P-C composite support strategy was used to improve the electrocatalytic performance of platinum nanoparticles for methanol, ethanol, ethylene glycol and formic acid, and to control the ratio of Cu_3P to C, it was found that when the mass ratio of Cu_3P to C was 1: 1, the electrocatalytic performance of the catalyst Pt- / C-C / Cu3P50% was the highest. It shows that the introduction of composite support can improve the catalytic activity of Pt catalyst. (3) the addition Fe2P is used to study the effect of Fe_2P on the electrocatalytic performance of Pt catalyst with different content of Fe_2P, in which the content of Fe_2P is less and the particle is smaller, which is different from the function of Cu_3P carrier. The effects of phosphates on the electrocatalytic activity of formic acid, methanol and ethanol in low content were analyzed. At present, as a new type of material, phosphates can enhance the electrocatalytic activity of fuel cell catalysts. When the content of Fe_2P is 5, the Pt catalyst has the best catalytic performance in the oxidation of methanol, ethanol and formic acid organic small molecule.
【學(xué)位授予單位】：太原理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TB383.1;TM911.4

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本文編號：1612450