以掃描式穿隧電子顯微鏡觀察氫氧化鎳於金(111)上結構及對甲醛氧化活性

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林廷駿(Ting-Chun Lin) 查詢紙本館藏

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論文名稱

以掃描式穿隧電子顯微鏡觀察氫氧化鎳於金(111)上結構及對甲醛氧化活性

相關論文

★ 岐狀結構材料在鋰電池的應用	★ Adsorption and Electrochemical Polymerization of Pyrrole on Au (100) Electrode as Examine by In Situ Scanning Tunneling Microscopy
★ Synthesis and Characterization of Cyclopentadithiophene (CDT) based Organic Photovoltaic and Pyrazine Contained Hole Transporting Small Molecules	★ 有機碘化物在金、銠、鉑(111)電極和有機二硫醇化物在鉑(111)電極的吸附結構
★ STM研究銥(111)上碘、一氧化碳和一氧化氮的吸附及銅(100)上鎳和鉛的沈積	★ 利用掃描式電子穿隧顯微鏡觀察鍍銅在鉑(111)及銠(111)電極表面
★ 使用in-situ STM和循環伏安儀研究銅和銀在碘修飾的鉑(100)電極之沈積過程	★ 利用in-situ STM觀察銅(100)電極上鉛與鎳的沉積過程
★ 利用in-situ STM觀察硫酸根、氧及碘在釕(001)電極和醋酸、間苯三酚在銠(111)電極的吸附結構	★ 掃描式電子穿隧顯微鏡及循環伏安法對有機碘化物在鉑(111)電極上的研究
★ 半導體碘化鉛薄膜在單結晶銠電極上的研究	★ 利用掃描式電子穿隧顯微鏡觀察汞薄膜在銥(111)電極上鹵素的吸附結構
★ 掃描式電子穿隧顯微鏡研究碘原子對汞在銥(111)、鉑(111)及銠(111)上沈積的影響	★ 掃描式電子穿隧顯微鏡對烷基及芳基硫醇分子在鉑(111)及金(111)上之研究
★ 掃描式電子穿隧顯微鏡研究一氧化碳、硫、硫醇分子及氯在釕(001)上的吸附結構	★ 硫氧化物及聚賽吩衍生物在金、鉑電極上之研究

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摘要(中)

甲醛為常見的室內空氣汙染物，其濃度過高時會對人體造成傷害，包含森林大火、菸草煙霧、汽車尾氣等等都會產生甲醛，故而檢測甲醛有其必要性存在，而電化學的氧化還原反應十分迅速，可即時偵測溶液中的甲醛濃度，故研究可以提升甲醛氧化活性的觸媒，不但可用於檢測甲醛濃度，也可去除溶液中的甲醛或當作燃料電池的一個方向。
　　此一研究以電化學方式將氫氧化鎳沉積於Au(111)電極表面，探討它對催化甲醛氧化的活性，並藉由掃描式穿隧電子顯微鏡輔助觀察其表面結構。實驗結果顯示Au(111)電極經1~2層氫氧化鎳修飾後，甲醛氧化電流從16.6提升至29.1 mA/cm2。在相同環境下，在Pt(111)上甲醛氧化電流為18.1 mA/cm2，顯示Ni/Au(111)電極大約有60%更高的活性。而從Koutecky–Levich方程式的計算結果得知，甲醛氧化反應轉移電子數在Au(111)和 Ni/Au(111)電極上，轉移電子數為0.94和2.6，經甲醛和[OH-]濃度變化的實驗結果推導出，甲醛氧化反應隨電極材料而不同，在金(111)為2HCHO+4OH-→2HCOO-+2H2O+H2+2e-，在Ni/Au(111)則是HCHO+3OH-→HCOO-+2H2O+2e-，原因可能是Ni的修飾導致其氫原子吸附自由能的改變。掃描式穿隧電子顯微鏡指出氫氧化鎳原子以六方最密堆積吸附於金電極上，於負電位區間其原子間距3 A，而正電位時其間距縮減為2.8 A，與文獻吻合，相對應電位主導之Ni(OH)2/NiOOH轉變。同時電極表面形貌在Ni(OH)2氧化為NiOOH後會由平坦轉變成三維球形顆粒。

摘要(英)

Formaldehyde (HCHO) is a commonly used reducing agent for electroless copper deposition in the electronic industry. It can be an intermediate produced in the oxidation of small organic molecules such as methanol. In addition to the notorious poisoning effect of carbon monoxide on the performance of direct methanol fuel cells, incomplete oxidation of methanol can lead to formaldehyde and formic acid, resulting in a lower cell voltage and less efficiency than the predicted. Formaldehyde is also known as a common air pollutant, which comes from forest fires, tobacco smoke, automobile exhaust, etc. It is harmful to human body above a certain concentration.
　　In this study, nickel hydroxide was electrodeposited on the surface of Au(111) electrode to fabricate a composite electrode, which has been used to catalyze the oxidation of formaldehyde. Voltammetric results show that the oxidation current of HCHO at bare and nickel hydroxide modified Au(111) electrodes have peak current densities of 16.6 and 29.1 mA/cm2, as compared with 18.1 mA/cm2 observed at Pt(111). The nickel-modified Au(111) has about 60% higher activity than Pt(111). The Koutecky–Levich plots were constructed from the results of rotating disk electrodes of Au(111) and Ni/Au(111), yielding a total number of electron of 0.9 and 2.64. These results imply that the oxidation of HCHO at Au(111) electrode is 2HCHO+4OH-→2HCOO-+2H2O+H2+2e-,at Ni/Au(111) electrode is HCHO+3OH-→HCOO-+2H2O+2e-. STM shows that the surface morphology of the Ni film changed from smooth to rough structures with more positive potentials. It is possible to obtain atomic resolution images showing that the nickel hydroxide supported by Au(111) has a hexagonal close packed atomic structure with an interatomic distance of 3 A in the negative potential region and transforms to a more closely packed lattice with a 2.8 A in-plane distance in the positive potential domain.

關鍵字(中)

★ 電化學
★ 甲醛氧化
★ 金(111)

關鍵字(英)

論文目次

摘要 i
Abstract ii
誌謝 iii
目錄 iv
圖目錄 v
表目錄 viii
第一章、緒論 1
1-1 甲醛介紹 1
1-2 氫氧化鎳特性及相關文獻回顧 1
1-3 Koutecky–Levich 方程式 2
1-4 衰減全反射式表面增強紅外光譜 3
1-5 甲醛氧化相關文獻 5
第二章、實驗部分 12
2-1 藥品部分 12
2-2 氣體部分 12
2-3 金屬部分 13
2-4 儀器設備 13
2-5 實驗步驟 16
第三章、結果與討論 23
3-1 氫氧化鎳於Au(111)電極之電化學特性 23
3-1-1、循環伏安圖 23
3-1-2、 STM圖 24
3-1-3、 XPS元素分析 26
3-2 甲醛氧化反應 39
3-2-1、 Au(111)電極之甲醛氧化 39
3-2-2、 Ni(111)電極之甲醛氧化 41
3-2-3、修飾氫氧化鎳Au(111)電極之甲醛氧化 41
第四章、結論 77
第五章、參考文獻 78

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指導教授

姚學麟

審核日期

2018-8-15

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