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

林祐霆(Lin You-Ting)

指導教授 ： 陳家俊

國立臺灣師範大學/理學院/化學系/碩士(2020年)

https://doi.org/10.6345/NTNU202000668

摘要

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。

關鍵字

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

並列摘要

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.

並列關鍵字

gold nanorods ； gold nanobipyramids ； Au/Ag-core/shell structure ； galvanic replacement reaction ； nanozappers ； hydrogen evolution reaction

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