| 研究生: |
吳佳芸 Wu, Chia-Yun |
|---|---|
| 論文名稱: |
以電沉積法製備鈀金合金薄膜及其甲醇電氧化催化特性之探討 Studies of PdAu alloy thin film via electrodeposition and its catalytic performance for methanol electro-oxidation |
| 指導教授: |
黃守仁
Whang, Thou-Jen |
| 學位類別: |
碩士 Master |
| 系所名稱: |
理學院 - 化學系 Department of Chemistry |
| 論文出版年: | 2017 |
| 畢業學年度: | 105 |
| 語文別: | 中文 |
| 論文頁數: | 170 |
| 中文關鍵詞: | 電沉積 、鈀金合金薄膜 、三乙醇胺 、退火熱處理 、甲醇電氧化 |
| 外文關鍵詞: | Co-electrodeposition, PdAu alloy thin film, complexing agent triethanolamine, Annealing, Methanol oxidation reaction |
| 相關次數: | 點閱:152 下載:0 |
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本實驗利用定電位電沉積的方法,在鍍有銦錫氧化物的導電玻璃(ITO Glass)上製備鈀金合金薄膜,並探討其薄膜性質與應用在甲醇電氧化上的性質比較。對於合金薄膜的製備方法,本實驗改變參數分別為:電沉積溶液中的鈀金離子的組成比例、電沉積電位、電沉積溶液中添加不同濃度之錯合劑三乙醇胺(TEA)、薄膜沉積時間與薄膜退火熱處理。
對於薄膜的晶型結構、元素組成、表面形貌與元素化學態性質,分別以X射線繞射分析儀(XRD)、能量分散式光譜分析儀(EDS)、掃描式電子顯微鏡(SEM)與X射線光電子能譜儀(XPS)進行量測。而甲醇電氧化效率與穩定性的探討,本實驗選用鹼性甲醇溶液,並利用循環伏安法(CV)和定電位電解法(CA)進行分析。
由晶面分析與表面形貌得知,加入錯合劑三乙醇胺會使Pd特徵峰具有寬化的現象,平均粒徑減小,並且粒子會呈現均勻分散的情況,得到較為均勻的鍍層。根據甲醇催化性質量測,當電沉積溶液中添加60 mM三乙醇胺,其沉積電位為-0.5 V時製備之鈀金合金薄膜整體電氧化效率與穩定性最佳,其中以電沉積溶液中金屬離子溶液比(Pd2+: Au3+)為4:1甲醇電氧化效率相對較佳,電流密度可達7.994 mA cm-2。而在退火熱處理的部分,Pd金屬在高溫環境下易於與氧分子進行反應形成Pd氧化物,使Pd失去催化甲醇之活性,因此薄膜甲醇電氧化效率大幅下降。
This experiment mainly focuses on the properties of methanol oxidation reaction (MOR) on PdAu alloy. In this work, PdAu thin films were co-electrodeposited on ITO glass substrates with different deposition conditions: metal ion precursor concentration ratio, the complexing agent triethanolamine(TEA) addition and thermal annealing treatment. The crystallinity of PdAu alloys was shown by X-ray diffractometer (XRD). The morphology of film surface was analyzed by scanning electron microscopy (SEM). The element composition of alloys were analyzed by energy-dispersive X-ray analysis (EDX) and X-ray photoelectron spectrometer (XPS). The electrochemical properties were tested by cyclic voltammetry (CV) and chronoamperometry (CA).
As a result, the electrochemical test indicated that binary PdAu alloys increased the efficiency of MOR. Moreover, the complexing agent TEA could not only enhance uniformity, stability and performance of PdAu alloy films, but lower the deposition potential while electrodepositing. The thermal annealing treatment resulted in the oxidation of Pd, degrading the MOR performance.
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