本文選題：直接甲醇燃料電池(DMFC)　切入點：氧還原反應(yīng)(ORR)　出處：《南京航空航天大學(xué)》2017年碩士論文

【摘要】：直接甲醇燃料電池(DMFC)作為一種清潔、高效以及便捷的新型能源,為研制便攜式移動能源創(chuàng)造了可能,受到了世界各國的廣泛關(guān)注。然而陰極氧還原催化劑作為一個難以攻克的瓶頸阻礙了其發(fā)展,這是由于陰極催化劑包含Pt、Pd等貴金屬,其價格不但昂貴還難以承受甲醇以及電解質(zhì)的腐蝕。目前,通過熱解處理得到非貴金屬M-N_x-C催化劑因氧還原催化性能良好,同時因以碳為載體而具有優(yōu)異的耐甲醇性能以及電化學(xué)穩(wěn)定性受到了廣泛的關(guān)注。本文以金屬有機骨架(MOF)作為前驅(qū)體引入M-N_x位點,以新型二維平面碳材料──石墨烯作為碳載體,制備了一系列的M-N_x-rGO催化劑,并對其進行了多種物理表征以及氧還原性能測試。主要研究內(nèi)容以及結(jié)論如下:(1)通過Fe或者Co金屬鹽提供M-N_x-rGO催化劑中的金屬,苯并咪唑為氮源,制備了一系列的M-N_x-rGO或者二元M-N_x-rGO催化劑,通過TEM、SEM、拉曼光譜、紅外光譜、比表面積以及孔徑測試、XRD、XPS等測試表明了廣泛認可的M-N_x活性位點不僅存在于石墨烯邊緣,而是很可能存在于層間,進一步提高了其氧還原催化性能。(2)通過改變制備條件得到一系列的M-N_x-rGO催化劑,探討反應(yīng)溫度、rGO添加量、熱解溫度以及金屬比對M-N_x-rGO催化劑氧還原催化性能的影響,最終通過LSV測試確定M-N_x-rGO催化劑最佳氧還原性能的制備條件。(3)對得到的氧還原性能最佳的M-N_x-rGO催化劑和Pt/C催化劑進行一系列的電化學(xué)測試,對比制備的M-N_x-rGO催化劑與Pt/C催化劑在氧還原催化性能、耐甲醇性能以及電化學(xué)穩(wěn)定性的優(yōu)劣。本論文以N,N二甲基甲酰胺(DMF)為溶劑,溶劑熱法制備了一系列M-N_x-rGO氧還原催化劑,對所制得的催化劑結(jié)構(gòu)進行了一定的研究,并探究了影響M-N_x-rGO氧還原催化性能的幾個因素。為M-N_x-C的繼續(xù)深入研究以及廣泛應(yīng)用于商業(yè)化生產(chǎn)提供了一定的借鑒依據(jù)。
[Abstract]:As a clean, efficient and convenient new energy source, DMFChas made it possible to develop portable mobile energy. However, cathodic oxygen reduction catalyst is a bottleneck that is difficult to overcome, which is due to the fact that the cathode catalyst contains precious metals such as PTO PD. It is not only expensive, but also difficult to withstand the corrosion of methanol and electrolyte. At present, the non-noble metal M-N_x-C catalyst has good catalytic performance due to oxygen reduction through pyrolysis. At the same time, due to the excellent methanol resistance and electrochemical stability due to carbon as the carrier, the metal-organic skeleton (MOF) was used as the precursor to introduce the M-N_x site. A series of M-N_x-rGO catalysts were prepared using a new two-dimensional planar carbon material, graphene, as a carbon carrier. The main contents and conclusions are as follows: (1) the metal in M-N_x-rGO catalyst was supplied by Fe or Co metal salts, and benzimidazole was used as nitrogen source. A series of M-N_x-rGO or binary M-N_x-rGO catalysts were prepared. The results of Tem, Raman, IR, specific surface area and pore size measurements showed that the widely recognized active sites of M-N_x not only existed at the edge of graphene, but also at the edge of graphene. A series of M-N_x-rGO catalysts were obtained by changing the preparation conditions, and the amount of RGO was discussed. Effects of pyrolysis temperature and metal ratio on the catalytic performance of M-N_x-rGO catalyst for oxygen reduction. Finally, the preparation conditions of the best oxygen reduction performance of M-N_x-rGO catalyst were determined by LSV test. (3) A series of electrochemical tests were carried out on the M-N_x-rGO catalyst and Pt/C catalyst, which had the best oxygen reduction performance. In this paper, a series of M-N_x-rGO oxygen reduction catalysts were prepared by solvothermal method, and their catalytic performance, methanol resistance and electrochemical stability were compared with those of the prepared M-N_x-rGO catalysts. The structure of the prepared catalyst was studied and several factors affecting the catalytic performance of M-N_x-rGO oxygen reduction were investigated. The results provided a reference for the further study of M-N_x-C and its wide application in commercial production.
【學(xué)位授予單位】：南京航空航天大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O643.36;TM911.4

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本文編號：1667778