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研究生: 林祐霆
Lin, You-Ting
論文名稱: 空間控制的三金屬奈米捕光器合成用於電漿增強的產氫反應
Synthesis of Spatial Controlled Trimetallic Nanozappers for Plasmon Boosted Hydrogen Evolution Reaction
指導教授: 陳家俊
Chen, Chia-Chun
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2020
畢業學年度: 108
語文別: 中文
論文頁數: 51
中文關鍵詞: 金奈米棒金奈米雙三角錐金/銀-核/殼結構賈凡尼置換反應奈米 捕光器產氫反應
英文關鍵詞: gold nanorods, gold nanobipyramids, Au/Ag-core/shell structure, galvanic replacement reaction, nanozappers, hydrogen evolution reaction
DOI URL: http://doi.org/10.6345/NTNU202000668
論文種類: 學術論文
相關次數: 點閱:205下載:12
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氫是宇宙中含量最多的元素,同時也是能量密度最高且乾淨的能源,因此光催化產氫反應(HER)成為近年來熱門的研究議題,貴金屬奈米材料通常具有優異的催化活性,但高昂的成本限制了其發展,因此低成本、高活性的催化材料開發勢在必行。本實驗利用晶種成長法,以兩種不同的界面活性劑,溴化十六烷基三甲銨(CTAB)與檸檬酸鈉(Na3CA)合成晶種,控制生長條件合成出尺寸相近的金奈米棒(AuNRs)與金奈米雙三角錐(AuNBPs),再將金奈米棒與金奈米雙三角錐分散於氯化十六烷基三甲銨(CTAC)的環境下,加入硝酸銀(AgNO3)及弱還原劑抗壞血酸(AA),將銀離子還原在金奈米粒子表面,形成金/銀-核/殼結構,利用賈凡尼置換反應,將鉑與銀進行置換還原至金/銀-核/殼結構表面,合成出三金屬奈米補光器。以TEM圖型研究此奈米結構的變化與差異,吸收光譜的調控可以從可見光到近紅外光的範圍。透過能量色散X射線譜元素面分析確認元素分布情形,以及使用感應偶合電漿質譜儀(ICP-MS)進行元素定量分析。將這三金屬奈米補光器(0.0192毫克的鉑負載量)應用於光催化產氫反應,照光後過電位降低約0.045 V。證明我們的三金屬奈米補光器有優異的光催化活性。

Hydrogen is the most abundant element in the universe, and it is also a clean energy with the highest specific energy. Recently, photocatalytic hydrogen evolution reaction (HER) has become a popular study. Noble metal nanomaterials have excellent catalytic activity, but their potential and application are limited by high cost. Therefore, there is an urgent need to develop low-cost and high-activity catalytic materials. In this work, two different surfactants, cetyltrimethylammonium bromide (CTAB) and sodium citrate, were used to synthesize the seed solutions for the further controlled growth of gold nanorods (AuNRs) and gold nanobipyramids (AuNBPs) with similar size. The as-prepared AuNRs and AuNBPs were dispersed into mixture containing CTAC and silver nitrate, and subsequently the weak reduction agent ascorbic acid was added to reduce silver ions onto the surface of gold nanoparticles to form the Au/Ag-core-shell nanostructures. For the synthesis of trimetallic nanozappers, galvanic replacement reaction was applied to replace the Ag atoms on the Au/Ag-core/shell nanostructures with the Pt ions. The shape evolution of the trimetallic nanozappers was observed by TEM images, and the corresponding UV-Vis absorption can be adjusted from visible to near-infrared range. Element distribution and element quantitative analysis were confirmed by energy-dispersive X-ray spectroscopy mapping and inductively coupled plasma mass spectrometry, respectively. Applying the synthesized trimetallic nanozappers (only contain 0.0192 mg Pt) to photocatalytic HER, the overpotential dropped significantly to 0.045 V under light irradiation. Our results show that the usage of trimetallic nanozappers has excellent plasmon enhanced photocatalytic activity.

目錄 摘要 I Abstract III 目錄 IV 圖表目錄 VII 第一章 緒論 1 1-1 奈米技術的發展 1 1-2 奈米材料的製作 3 1-3 金屬奈米材料的特性 4 1-4 金屬奈米材料的應用 5 第二章 文獻回顧及研究動機 7 2-1 金奈米棒與金奈米雙三角錐 7 2-2 金/銀-核/殼結構 9 2-3 Galvanic Replacement Reaction 10 2-4 Hydrogen Evolution Reaction 11 2-5 研究動機 14 第三章 實驗藥品儀器及實驗步驟 15 3-1 實驗藥品 15 3-2 實驗測量儀器 16 3-2-1 紫外光-可見光-近紅外光分光光譜儀(UV-Visble-Near IR Spectrophotometer)16 3-2-2 穿透式電子顯微鏡(Transmission Electron Microscopy, TEM) 17 3-2-3 超高解析冷槍場放射型掃描式電子顯微鏡TE Detector 18 3-2-4 高速離心機(Universal Centrifuges) 20 3-2-5 恆溫循環水槽 21 3-3 實驗步驟 22 3-3-1 Synthesis of Gold Nanorods(AuNRs) 22 3-3-2 Synthesis of Gold Nanobipyramids(AuNBPs) 23 3-3-3 Silver Overgrowth on Gold Nanoparticles 24 3-3-4 Galvanic Replacement Reaction 25 3-3-5 Hydrogen Evolution Reaction 26 3-3-6 ICP-MS樣品前處理 27 第四章 結果與討論 28 4-1 金奈米棒與金奈米雙三角錐 28 4-1-1 金奈米棒 28 4-1-2 金奈米雙三角錐 29 4-2 金/銀-核/殼結構 30 4-2-1 金奈米棒/銀-核/殼結構 30 4-2-2 金奈米雙三角錐/銀-核/殼結構 31 4-3 估算金/銀-核/殼結構之銀含量 32 4-4 Galvanic Replacement Reaction 34 4-4-1 金奈米棒/銀-核/殼結構之置換反應 34 4-4-2金奈米雙三角錐/銀-核/殼結構之置換反應 36 4-5 Hydrogen Evolution Reaction 38 4-6 元素分布及定量分析 44 4-6-1 能量色散X射線譜元素面分析 44 4-6-2 元素定量分析 45 第五章 結論 46 參考文獻 47

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