研究生: |
彭怡貞 Yi-Jhen Peng |
---|---|
論文名稱: |
金屬混合氧化物擔載Pt觸媒製備參數對其氫氣氧化反應的CO耐受性探討 Preparation of 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: |
黃炳照
Bing-Joe Hwang 王丞浩 Chen-Hao Wang 林修正 Andrew S. Lin |
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: | 2016 |
畢業學年度: | 104 |
語文別: | 中文 |
論文頁數: | 165 |
中文關鍵詞: | 金屬混合氧化物 、雙離子摻雜 、水熱法 、氫氣氧化反應 |
外文關鍵詞: | Metal oxide, Dual ion-doping, Hydrothermal process, Hydrogen oxidation reaction |
相關次數: | 點閱:241 下載:2 |
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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PEMFC操作條件下會有碳腐蝕現象發生,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Ti0.7Ru0.3O2 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:載體還原性前處理、雙離子摻雜與Ru添加方式,並比較Ti0.7Ru0.3O2、Zr0.7Ru0.3O2與W0.7Ru0.3O2擔載觸媒之特性。
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 onset potential與氫氣氧化反應(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,發現以磷摻雜的40Pt/P-Ti0.7Ru0.3O2-b12 與40Pt/W0.7Ru0.3O2觸媒具有較商用20Pt10Ru/C與40Pt/Ti0.7Ru0.3O2觸媒高的抗CO能力、氫氣氧化活性與穩定性。
Proton exchange membrane fuel cells (PEMFCs) are expected to have enormous power for both mobile and stationary applications (e.g., automotive, portable, electronics, etc.). 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 durability and CO tolerance of anodic catalysts, mixed-oxide supports are examined in this study. A simple hydrothermal process is applied to synthesize supports and the influences of preparation parameters are examined, including pretreatment conditions, dual ion-doping, sequences of Ru inclusion, and changes of M in M0.7Ru0.3O2.
Pt loading is prepared by EG method. XRD results show that the prepared 40% Pt/P-Ti0.3Ru0.7O2 contains Pt particle size of 3-4 nm, similar with commercial PtRu/C catalysts. CO stripping and hydrogen oxidation reaction (HOR) under H2 with 100 and 250 pm CO are examined. The results indicate that 40Pt/P-Ti0.7Ru0.3O2-b12 and 40Pt/W0.7Ru0.3O2 catalysts exhibit improved CO tolerance, intrinsic activity and durability comparing to commercial PtRu/C and homemade 40% Pt/Ti0.7Ru0.3O2 catalysts.
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