電沉積法制備鈷硒化合物及其氧還原性能研究
發(fā)布時(shí)間:2018-04-25 22:19
本文選題:燃料電池 + 氧還原催化劑; 參考:《哈爾濱工業(yè)大學(xué)》2017年碩士論文
【摘要】:燃料電池是一種通過(guò)電化學(xué)反應(yīng),直接將儲(chǔ)存在燃料中的化學(xué)能轉(zhuǎn)換為電能的綠色發(fā)電裝置。而人們一直在尋找可以替代Pt的非貴金屬燃料電池陰極催化劑,以解決成本高的問(wèn)題。Co-Se化合物對(duì)氧還原反應(yīng)具有較強(qiáng)的催化能力。電沉積法合成Co-Se化合物可以將催化劑直接電沉積到膜電極的活性位點(diǎn)上,能夠極大地提高催化劑的利用率。而且關(guān)于電沉積法用于燃料電池氧還原催化劑的研究比較少,所以本文對(duì)電沉積Co-Se化合物氧還原催化劑進(jìn)行了研究。首先采用恒電勢(shì)電沉積法在銅片上電沉積Se薄膜,在以主鹽為SeO2的水溶液中研究了電沉積Se的電化學(xué)行為,結(jié)果表明Se的沉積過(guò)程分三步進(jìn)行,先發(fā)生Se的四電子還原,再發(fā)生Se的六電子還原,最后在電極表面發(fā)生化學(xué)還原。探究了沉積電位、主鹽濃度、溫度、pH對(duì)電沉積Se薄膜形貌和結(jié)構(gòu)的影響,分別在20 ℃和40 ℃時(shí)得到了具有單斜晶系結(jié)構(gòu)和六方晶系結(jié)構(gòu)的紅硒和灰硒。采用恒電勢(shì)電沉積法在碳紙上直接電沉積Co-Se化合物作為氧還原催化劑,首先對(duì)Co-Se的電沉積過(guò)程進(jìn)行了研究,分析了Co-Se在水溶液中的共沉積規(guī)律,探究不同掃速對(duì)Co-Se共沉積循環(huán)伏安行為的影響,分析了電極過(guò)程的控制步驟。通過(guò)研究主鹽濃度、主鹽濃度比、沉積電位、溫度等工藝條件,得到富硒的具有方硒鈷礦結(jié)構(gòu)的CoSe2化合物,并對(duì)其形貌、組成、結(jié)構(gòu)及氧還原性能進(jìn)行研究。結(jié)果表明,在堿性或酸性電解液中均具有良好的氧還原催化活性和催化穩(wěn)定性。該方法制備的CoSe2化合物用作燃料電池氧還原催化劑具有成本低、催化性能好、穩(wěn)定性高等優(yōu)點(diǎn),有望在商用燃料電池中應(yīng)用。
[Abstract]:Fuel cell is a kind of green power plant which directly converts the chemical energy stored in the fuel into electric energy by electrochemical reaction. In order to solve the problem of high cost, Co-Se compounds have strong catalytic ability for oxygen reduction. The synthesis of Co-Se compounds by electrodeposition can directly electrodeposit the catalyst onto the active site of the membrane electrode, which can greatly improve the utilization rate of the catalyst. And there are few researches on the electrodeposition of oxygen reduction catalysts for fuel cells, so the electrodeposition of oxygen reduction catalysts for Co-Se compounds has been studied in this paper. At first, the electrodeposition of se thin films on copper substrates was carried out by potentiostatic electrodeposition. The electrochemical behavior of se was studied in aqueous solution with the main salt as SeO2. The results showed that the deposition process of se was divided into three steps, and the reduction of se by four electrons was first observed. The six electron reduction of se and the chemical reduction of se on the surface of the electrode occurred again. The effects of deposition potential, concentration of main salt and temperature and pH on the morphology and structure of se films were investigated. Red selenium and grey selenium with monoclinic and hexagonal structure were obtained at 20 鈩,
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