研究生: |
黃國晏 Guo-Yan Huang |
---|---|
論文名稱: |
鎢釕混合氧化物擔載Pt觸媒製備參數對其氫氣氧化反應的CO耐受性探討 Preparation of Tungsten Ruthenium mixed oxide supported Pt catalysts for CO tolerance in Hydrogen Oxidation Reaction |
指導教授: |
林昇佃
Shawn D. Lin |
口試委員: |
林修正
Andrew S. Lin 蘇威年 Wei-Nien Su 黃炳照 Bing-Joe Hwang |
學位類別: |
碩士 Master |
系所名稱: |
工程學院 - 化學工程系 Department of Chemical Engineering |
論文出版年: | 2018 |
畢業學年度: | 106 |
語文別: | 中文 |
論文頁數: | 115 |
中文關鍵詞: | 金屬混合氧化物 、陽離子摻雜 、水熱法 、氫氣氧化反應 |
外文關鍵詞: | Metal mixed oxide, cation-doping, hydrothermal process, hydrogen oxidation reaction |
相關次數: | 點閱:272 下載:4 |
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氫能時代的來臨,將對照驗證質子交換薄膜燃料電池(PEMFC)技術的發展成熟度,目前PEMFC電極觸媒主要是以碳當作載體,利用碳載體的高導電性與高比表面積以使Pt可以均勻分散,但在操作過程發生的碳腐蝕現象,會導致Pt觸媒活性下降,並降低PEMFC的效能。本研究目的為探討非碳載體之金屬混合氧化物陽極反應觸媒,以提升觸媒穩定性,並提升觸媒抗CO毒化能力,以實驗室先前水熱法合成的W0.7Ru0.3O2 載體為基礎,進一步測試製備參數對觸媒的影響,所測試的參數包括:不同晶相氧化鎢載體、Ru陽離子摻雜形成不同鎢釕比例載體與不同載體鍛燒溫度,最後進行製作流程優化。
研究結果顯示以EG法自製40%Pt氧化物擔載觸媒可獲得與商用PtRu/C觸媒相近的Pt粒徑(3-4奈米),以CO-stripping測試中CO起始氧化電位與峰電位,和氫氣氧化反應(HOR)在純氫、100和250ppm CO環境下的旋轉圓盤電極分析與定電位分析,發現優化流程製得的40Pt/W5Ru5-N12-c300與40Pt/W7Ru3-N12-c300觸媒具有比擬商用20Pt10Ru/C觸媒的良好抗CO能力、氫氣氧化活性與穩定性。
Proton exchange membrane fuel cells (PEMFCs) are expected to have enormous potential for both mobile and stationary applications. Carbon supports are mainly used in electrocatalysts for fuel cells because of good electron conductivity and high surface area that may leads to good dispersion of active Pt particles. However, carbon corrosion under operating conditions of PEMFCs becomes a concern which can cause deterioration in the performance of Pt catalysts. To enhance the durability and the CO tolerance of anodic catalysts, mixed-oxide supports are examined in this study. A simple hydrothermal process is applied to synthesize mixed W-Ru oxide supports and the influences of preparation parameters are examined, including Tungsten oxide phase, Tungsten Ruthenium ratio, and pretreatment temperature, and subsequently the preparation procedure is optimized.
Pt loading is prepared by EG method. XRD results show that the prepared 40wt%Pt/W5Ru5-N12-c300 contains Pt particle size of 3-4 nm. CO stripping and hydrogen oxidation reaction (HOR) with 100 and 250 ppm CO are examined. The results indicate that 40Pt/W5Ru5-N12-c300 and 40Pt/W7Ru3-N12-c300 catalysts exhibit improved CO tolerance, intrinsic activity and durability comparing to the other prepared catalysts. The overall performance is comparable with commercial 20Pt10Ru/C catalysts.
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