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研究生: 黃馨瑩
Huang, Xin-Ying
論文名稱: 合成不同形貌的銀釕奈米粒子並藉由表面電漿共振去趨動固氮反應
Synthesize Ag-Ru nanocrystals with different morphology for the plasmon-induced N2 fixation
指導教授: 吳欣倫
Wu, Hsin-Lun
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: 2021
畢業學年度: 109
語文別: 中文
論文頁數: 47
中文關鍵詞: 銀釕奈米粒子表面電漿共振伽凡尼置換反應光催化固氮反應
外文關鍵詞: Ag-Ru nanocrystals, surface plasmon resonance, galvanic replacement reaction, photocatalysis, nitrogen fixation reaction
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  • 本篇實驗主要討論的方向有三個,第一,是利用磊晶生長的方法來控制雙金屬奈米粒子的晶體結構,來合成出具有面心立方結構的銀釕奈米粒子;第二,我們發現不同的釕金屬前驅物會造成銀釕奈米粒子的形貌不同,乙酰丙酮釕(Ru(acac)3)傾向與銀奈米粒子進行磊晶生長形成實心結構,而三氯化釕(RuCl3)則是傾向與銀奈米粒子進行伽凡尼置換反應形成中空結構,我們推測是因為不同的釕金屬前驅物相對於銀奈米粒子的還原電位不同所造成的。此外,更進一步的利用三氯化釕的濃度來控制銀釕奈米粒子的形貌結構;第三,則是將具有表面電漿共振性質且不同形貌的銀釕奈米粒子,照射可見光範圍的光,使其產生熱電子去趨動固氮反應,並用吲哚酚藍試劑檢測氨的產率。

    In this study, we use the epitaxial growth method to synthesize the Ag-Ru nanocrystals with a face-centered cubic structure. We found that the ruthenium(Ru) precursors caused different morphology of the Ag-Ru nanocrystals. A core-shell structure was formed by using the ruthenium (III) acetylacetonate (Ru(acac)3), while a hollow structure was formed by using the ruthenium (III) chloride (RuCl3), when reacted with the Ag nanocrystals. We supposed that the results were attributed to potential difference of the Ru precursors relative to the Ag nanocrystals. Furthermore, the concentration of the RuCl3 could be used to control the morphology of the Ag-Ru nanocrystals. Finally, different morphology of the Ag-Ru nanocrystals with the localized surface plasmon resonance property were used to drive the nitrogen fixation reaction by hot electrons under illuminating with visible light. The indophenol blue method were used to detect the yield of ammonia.

    第一章介紹 1 1-1哈伯法製氨 1 1-2光催化劑的發展 2 1-3表面電漿共振原理 3 1-3-1銀做為熱電子提供者 5 1-4新型材料的反應機制 6 1-4-1釕吸附氣體的選擇性 7 1-5控制晶體結構 8 1-5-1磊晶生長 10 1-5-2擴散速率與還原速率 12 1-6利用共還原反應製備合金 14 1-7利用伽凡尼置換反應製備合金 16 1-8實驗動機 18 1-9參考資料 19 第二章合成銀釕奈米粒子 21 2-1介紹 21 2-2儀器 22 2-3藥品 23 2-4合成銀奈米立方體之實驗步驟 24 2-4-1鑑定銀奈米立方體 25 2-5合成銀釕核殼奈米粒子之實驗步驟 26 2-5-1鑑定銀釕核殼奈米粒子 27 2-6比較RuCl3與Ru(acac)3差別之實驗步驟 30 2-6-1還原電位的差異 31 2-7控制RuCl3濃度改變中空結構比例的反應步驟 32 2-7-1中空結構的鑑定 33 2-8探討氯離子對於實驗結果的影響 38 2-9固氮反應的實驗步驟 42 2-9-1配置吲哚苯酚試劑以及變色原理 42 2-9-2固氮反應的結果與討論 44 2-10結論 46 2-11參考資料 47

    1-9 參考資料
    (1) Erisman, J. W. et al., Nat. Geosci. 2008, 1, 636.
    (2) Soloveichik, G. Nat. Catal. 2019, 2, 377.
    (3) Humphreys, J. et al., Adv. Energy Mater. 2021, 2, 2000043.
    (4) Mitsushima, S. et al.,: Chapter 11 - Role of Hydrogen Energy Carriers. In Fuel Cells and Hydrogen; Hacker, V. et al., Eds.; Elsevier, 2018; 243.
    (5) Kiehl, J. T. et al., Bull Am Meteorol Soc. 1997, 78, 197.
    (6) MacFarlane, D. R. et al., Joule 2020, 4, 1186.
    (7) Chu, K. et al., J. Mater. Chem. A 2020, 8, 5200.
    (8) Chu, K. et al., J. Mater. Chem. A 2020, 8, 7117.
    (9) Li, Q. et al., J. Mater. Chem. A 2020, 8, 16195.
    (10) Schrauzer, G. N. et al., J. Am. Chem. Soc. 1977, 99, 7189.
    (11) Mou, H. et al., ACS Appl. Mater. Interfaces 2019, 11, 44360.
    (12) Liu, S. et al., ACS Sustain. Chem. Eng. 2019, 7, 6813.
    (13) Zhao, Z. et al., ChemComm 2019, 55, 7171.
    (14) Hu, C. et al., J. Am. Chem. Soc. 2019, 141, 7807.
    (15) Hou, T. et al., ACS Energy Lett. 2020, 5, 2444.
    (16) Kravets, V. G. et al., Chem. Rev. 2018, 118, 5912.
    (17) Zhang, J. et al., J. Phys. D 2012, 45, 113001.
    (18) Zhang, Y. et al., Chem. Rev. 2018, 118, 2927.
    (19) Rycenga, M. et al., Chem. Rev. 2011, 111, 3669.
    (20) Xia, Y. et al., Angew. Chem. Int. Ed. Engl. 2009, 48, 60.
    (21) Shipman, M. A. et al., Catal. Today 2017, 286, 57.
    (22) Mao, X. et al., J. Mater. Chem. A 2021, 9, 6575.
    (23) Yao, Y. et al., ACS Energy Lett. 2019, 4, 1336.
    (24) Niu, X. et al., J. Phys. Chem. Lett. 2020, 11, 9579.
    (25) Medford, A. J. et al., ACS Catal. 2017, 7, 2624.
    (26) Zhang, Q. et al., Nat. Commun. 2018, 9, 510.
    (27) Kusada, K. et al., J. Am. Chem. Soc. 2013, 135, 5493.
    (28) Zhao, M. et al., J. Am. Chem. Soc. 2019, 141, 7028.
    (29) Ye, H. et al., Nano Lett. 2016, 16, 2812.
    (30) Zhao, M. et al., Nano Lett. 2016, 16, 5310.
    (31) Chayen, N. E. Prog. Biophys. Mol. Biol. 2005, 88, 329.
    (32) Niu, W. et al., Nanoscale 2013, 5, 3172.
    (33) Tan, C. et al., Nat. Rev. Mater. 2018, 3, 17089.
    (34) Kum, H. et al., Nat. Electron. 2019, 2, 439.
    (35) Xia, Y. et al., J. Am. Chem. Soc. 2015, 137, 7947.
    (36) Zhang, Q. et al., Chem. Sci. 2019, 10, 5133.
    (37) Weng, G. et al., J. Mater. Sci. 2016, 51, 7678.
    (38) Millstone, J. E. et al., Nano Lett. 2008, 8, 2526.
    (39) Wiley, B. et al., Nano Lett. 2004, 4, 1733.
    (40) Gu, Y. et al., New J. Chem. 2016, 40, 7557.
    (41) Ghosh, S. et al., Chem. Rev. 2018, 118, 7804.
    (42) Chee, S. W. et al., Nat. Commun. 2017, 8, 1224.
    (43) Xia, X. et al., Adv. Mater. 2013, 25, 6313.
    (44) da Silva, A. G. M. et al., ChemComm 2017, 53, 7135.
    (45) Lin, S.-C. et al., J. Am. Chem. Soc. 2017, 139, 2224.

    2-11參考資料
    (1) Siekkinen, A. R. et al., Chem. Phys. Lett. 2006, 432, 491.
    (2) Zhang, Q. et al., Chem. Eur. J. 2010, 16, 10234.
    (3) Zhang, Q. et al., ACS Appl. Mater. Interfaces 2009, 1, 2044.
    (4) Wang, Y. et al., J. Am. Chem. Soc. 2013, 135, 1941.
    (5) Kusada, K. et al., J. Am. Chem. Soc. 2013, 135, 5493.
    (6) Morais, E. et al., Int. J. Photoenergy 2019, 2019, 3651603.
    (7) Zhao, Y. et al., Adv. Sci. 2019, 6, 1802109.
    (8) Zhao, X. et al., ChemComm 2018, 54, 13010.
    (9) Afkhami, A. et al., J Braz Chem Soc 2008, 19, 1546.
    (10) J. Michałowicz, W. D. Pol J Environ Stud 2007, 16, 347.
    (11) Zhu, Y. et al., Trends Analyt Chem 2019, 119, 115627.

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    2026-08-12公開
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