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  • 學位論文

製備鉑-二氧化鈰/碳甲醇氧化電催化劑與其性質分析

Preparation and Characterization of Pt-CeO2/C Electrocatalysts for Methanol Oxidation Reaction

指導教授 : 林正嵐

摘要


本研究主要目的為製備甲醇燃料電池 (Direct Methanol Fuel Cell, DMFC) 的鉑-二氧化鈰/碳電催化劑並對其性質進行分析研究。 利用多元醇還原法製備鉑-二氧化鈰/碳電催化劑並與商用鉑/碳電催化劑進行分析與比較。電催化劑所使用的碳載體 (XC-72)實驗前先利用氫氧化納水溶液進行鹼修飾或利用硝酸水溶液進行酸修飾,主要目的是為了改變碳載體表面結構而增加電催化劑上金屬或金屬氧化物的分散性。多元醇還原法是利用乙二醇為還原劑將鉑與二氧化鈰還原到碳載體表面而製備成高分散性的鉑-二氧化鈰/碳電催化劑。 本研究使用掃描式電子顯微鏡 (scanning electron microscope, SEM) 對電催化劑表面進行元素分析,分析結果顯示電催化劑表面鉑與二氧化鈰的實際值與理論值相當接近。穿透式電子顯微鏡 (transmission electron microscope, TEM) 結果顯示碳載體上的鉑與二氧化鈰分散的非常均勻,沒有任何聚集的情況發生。實驗結果顯示電催化劑上鉑的粒徑大約在3-4 nm 左右,與使用 X 光繞射分析儀 (X-ray diffractometer, XRD) 所計算出的粒徑大小相當吻合。 碳載體經由硝酸修飾再利用乙二醇還原法所製備的電催化劑 Pt-CeO2/ Ca 利用循環伏安法 (cyclic voltammetry, CV) 進行甲醇氧化反應 (MOR) 效能測試,實驗結果顯示電催化劑的 MOR效能為商用 Pt (E-TEK)/C電催化劑的 2.5 倍。利用計時安培法 (chronoamperometry, CA) 測試電催化劑的穩定性,實驗結果顯示電催化劑 Pt-CeO2/ C 的穩定性也比商用 Pt (E-TEK)/C電催化劑還要佳。 本研究對於製備電催化劑的方法、碳載體鹼或酸修飾或鉑與鈰在不同莫耳比下所製備出的電催化劑進行分析與比較,並將電催化劑的效能最佳化。

並列摘要


The research are the preparation and characterization of Pt-CeO2/C electrocatalysts for the methanol oxidation reaction (MOR) of a direct methanol fuel cell (DMFC).Pt-CeO2/C electrocatalysts have been synthesized by polyol method and compared with Pt/C (E-TEK) electrocatalysts. Carbon black (Vulcan XC-72) was pretreated with NaOH or HNO3 aqueous solution. A Polyol method is using ethylene glycol as the reducing agent to grows the Pt nanoparticles and CeO2 on the carbon black (CB), then get the Pt-CeO2/C nanocomposite electrocatalysts. Scanning electron microscopic (SEM) images with energy dispersive spectroscopic (EDS) reveal that the Pt and CeO2 contents in the samples are close to the nominal values. Transmission electron microscope (TEM) pictures showed a uniform distribution of platinum on the CB, and observed that the Pt nanoparticles diameter are around 3-4 nm almost close the result of consideration from X-ray diffraction (XRD). The Pt-CeO2/ Ca electrocatalysts by polyol method exhibit 2.5 times higher electrochemical activities for MOR in cyclic voltammetry (CV) experiments, compared with the Pt/C (E-TEK) electrocatalysts. The Pt-CeO2/C electrocatalysts also showed higher stability in chronoamperometry test (CA).In this report,we also compare the property of Pe/Ce molar ratio and the difference way to pretreat CB effect in the experience.

並列關鍵字

DMFC Ceria Electrocatalysts

參考文獻


[1] 衣寶廉, 燃料電池-原理與應用, 五南圖書出版公司 (2007)
[3] “DMFCs:From Fundamental Aspects to Technology Development”, Arico, A.S.; Srinivasan, S.; Antonucci, V.; Fuel Cells 2001, 1, 133.
[4] “On the role of Ru and Sn as promoters of methanol electro-oxidation over Pt”, Freelink, T.; Visscher, W. Surf. Sci. 1995, 335, 353.
[5] “Promotion of Carbon Supported Platinum-Ruthenium Catalyst for Electro-decomposition of Methanol”, Wang, K.W.; Huang, S.Y.; Yeh, C.T.; J. Phys. Chem. C 2007, 111, 5096.
[6] “Effect of heat treatment on PtRu/C catalyst for methanol electro-oxidation”, Xiong, L.; Manthiram, A.; Solid State Ionic 2005, 176, 385.

被引用紀錄


葉如玉(2014)。鉑/二氧化矽-碳黑甲醇氧化電催化劑之製備與性質分析〔碩士論文,淡江大學〕。華藝線上圖書館。https://doi.org/10.6846/TKU.2014.00302

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