本文選題：氧還原反應(yīng)　切入點(diǎn)：催化劑　出處：《重慶大學(xué)》2015年碩士論文

【摘要】：燃料電池因具有新穎、清潔、高效、可持續(xù)的特點(diǎn)而引起人們的廣泛關(guān)注,但陰極緩慢的的氧還原反應(yīng)(ORR)動力學(xué)是限制其大規(guī)模應(yīng)用的關(guān)鍵因素。迄今為止,用于氧還原反應(yīng)(ORR)的最有效和最廣泛的催化劑仍然是鉑。然而眾所周知,Pt系催化劑具有性價高、甲醇耐受性低和穩(wěn)定性有限等缺點(diǎn),這些都是新能源系統(tǒng)商業(yè)化的阻礙。因此,開發(fā)安全高效的非貴金屬代替催化劑是十分迫切的任務(wù)。研究發(fā)現(xiàn),TM-N/C催化劑,是一種很有希望的Pt/C催化劑的替代物。本論文以廣泛應(yīng)用的Vulcan XC-72為碳源,COCl2·6H2O為過渡金屬供體,創(chuàng)新性地提出直接化學(xué)還原法和氨水水熱摻氮法結(jié)合使用,制備出一系列的TM-N/C催化劑。實(shí)驗(yàn)討論了催化劑制備中各種制備條件對催化劑性能的影響,并利用LSV評價了所制備的TM-N/C催化劑的活性與商業(yè)Pt/C催化劑活性的差異。結(jié)果證明：利用氨水在水熱條件下對C材料進(jìn)行摻氮的方法是有效的,過渡金屬的參與、C載體的預(yù)先氧化處理對提高催化劑的性能所起的作用是十分重要的,水熱摻氮反應(yīng)的最佳反應(yīng)條件為180℃,9h,實(shí)驗(yàn)所制備的催化劑的峰電位與商業(yè)Pt/C催化劑相近。本論文還創(chuàng)新性地選取含豐富葉綠素的綠色植物葉片做為原材料,與C載體Vulcan XC-72和過渡金屬Fe、Co鹽混合研磨后進(jìn)行熱解處理制備菜葉系列催化劑�？疾炝藷峤庵懈魑锓N的比例、熱解的溫度和時間、過渡金屬的選擇和最佳含量等因素對催化劑性能的影響,并詳細(xì)表征了催化劑的電化學(xué)性能。結(jié)果表明菜葉做催化劑前驅(qū)體的方法是可行的。菜葉的酸浸脫鎂步驟、C載體的加入和過渡金屬的加入都能使催化劑的催化活性變得更優(yōu)。實(shí)驗(yàn)的最佳條件為酸浸除鎂24h,SWA:C=1, Fe wt.%=8%,900℃下熱解2h。并驗(yàn)證了菜葉催化劑中對催化劑活性起貢獻(xiàn)作用的是葉綠素。在堿性條件下,實(shí)驗(yàn)制備的最佳催化劑SWA+C+Fe-900-2h性能與商業(yè)Pt/C催化劑的催化性能相近。通過旋轉(zhuǎn)圓盤電極測得SWA+C+Fe-900-2h的轉(zhuǎn)移電子數(shù)為3.9接近Pt的4,循環(huán)穩(wěn)定性和耐甲醇性均優(yōu)于商業(yè)Pt/C催化劑。這兩種方法制備的TM-N/C催化劑對Pt替代催化劑的發(fā)展具有一定的參考價值。
[Abstract]:Fuel cell with new, clean, efficient and sustainable characteristics and aroused extensive attention, but the slow cathodic oxygen reduction reaction (ORR) dynamics is the key factor to limit its large-scale application. So far, for the oxygen reduction reaction (ORR) is the most effective and most widely used catalyst is still however platinum. As everyone knows, Pt catalyst has high stability and low methanol tolerance, limited and other shortcomings, these are hindering the commercialization of new energy systems. Therefore, the development of safe and efficient non noble metal catalyst instead of is a very urgent task. The study found that TM-N/C catalyst is a substitute for the Pt/C catalyst is very promising the. In this paper, the widely used Vulcan XC-72 as carbon source, COCl2 - 6H2O transition metal donor, creatively put forward the direct chemical reduction method and hydrothermal method with ammonia nitrogen doped with a series of preparation The TM-N/C catalyst. The experimental effects of preparation of catalyst preparation conditions on catalyst performance, and use LSV to evaluate the difference of the prepared TM-N/C catalyst activity and commercial activity of the Pt/C catalyst. The results showed that: the use of ammonia under hydrothermal conditions and methods on the C material in nitrogen doping is effective C, transition metal in the pre oxidation treatment of the carrier to improve the catalytic performance of the role is very important, the optimum reaction conditions of hydrothermal reaction of nitrogen doped is 180 DEG C, 9h, C and peak potential of commercial Pt/ catalyst experiment of the prepared catalysts are similar. This paper also creatively chooses green leaves of plants containing abundant chlorophyll as raw materials, and C vector Vulcan XC-72 and transition metal Fe, Co salt mixed grinding after preparation leaves series catalyst was studied. The pyrolysis process of each species in the proportion of thermal pyrolysis, solution The temperature and time, the influence factors of transition metal and the choice of the best content on the catalyst performance, and electrochemical performance of the catalyst were investigated in detail. The results show that the method leaves do catalyst precursor is feasible. The leaves of acid leaching of magnesium removal steps, C carrier addition and adding transition metal can make catalysis the activity of the catalyst becomes better. The optimum experimental conditions for acid leaching of magnesium 24h, SWA:C=1, Fe, wt.%=8%, 900 degrees 2h. and verify the pyrolysis contribution on the catalytic activity of catalyst in the leaves is chlorophyll. In alkaline conditions, the catalytic performance of SWA+C+Fe-900-2h catalyst and the best performance of commercial Pt/C catalyst was prepared. Similar. Number of electron transfer through the rotating disk electrode of SWA+C+Fe-900-2h was measured to be 3.9 to 4 of Pt, cycle stability and methanol resistance are better than that of commercial Pt/C catalyst. The two kinds of methods of preparation The TM-N/C catalyst has a certain reference value for the development of Pt substitute catalyst.

【學(xué)位授予單位】：重慶大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：O643.36;TM911.4

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