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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 楊吉水(Jye-Shane Yang) | |
dc.contributor.author | Ting-Wei Wu | en |
dc.contributor.author | 吳庭緯 | zh_TW |
dc.date.accessioned | 2021-06-15T12:26:03Z | - |
dc.date.available | 2025-08-20 | |
dc.date.copyright | 2020-09-22 | |
dc.date.issued | 2020 | |
dc.date.submitted | 2020-08-17 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/49910 | - |
dc.description.abstract | 金(I)錯合物獨有的”親金作用力”,可受外界刺激,如機械力、有機物蒸氣、熱及光等的影響而改變。親金作用力為金(I)離子與金(I)離子之間彼此透過非共價鍵所形成的作用力,距離大約為2.5~3.8埃。親金作用力的變化,往往可使放光有顏色上的變化,因此使金(I)錯合物被廣泛應用於刺激響應材料當中。 本實驗室過去發表了一系列以五苯荑為主體的刺激響應材料,主要可歸因於剛硬且H型結構的五苯荑基團。首先,其可有效阻止分子間的π-π堆疊,使分子於固態下有著良好的放光效率;此外,特殊的U型凹槽及V型凹槽,可於固態下提供各種不同的排列模式以及與客體分子發生超分子作用力,使放光顏色有許多變化。 在這篇論文中,我們合成一系列含五苯荑的金(I)-炔基錯合物,並修飾上不同的苯乙炔基配體。其中以最簡單的苯乙炔原型被命名為Ph;以及延伸共軛長度的Naph及An;修飾不同對位取代的苯乙炔,命名為OMe、CN及CF3。我們觀察其受刺激後之放光行為,並透過光譜、晶體結構以及拉曼光譜提出合理機制。 我們的結果顯示全部的錯合物都具有力致放光變色的響應,主要歸因於研磨可使親金作用力增強,進一步使放光紅移;又或者開啟/減少激發雙體放光,使得光譜紅移/藍移。 我們還發現對位取代系列的錯合物對苯胺小分子具放光響應,形成激發複合體放光,且隨著錯合物的缺電子性增加,紅位移的程度會隨之提升;透過與晶體結構的連結,我們歸納出孔洞結構為一重要的因素。 此外,對位取代系列錯合物的晶體,通過紫外光的照射可使放光紅移至橘紅色,然而整體的放光效率變差;由於循序漸進的紅移,會經過一白色放光的過渡狀態。經光照後,親金作用力增強,生成以四核金原子團簇為主導的消光團,導致單體形式放光經由能量轉移淬滅為可能的機制。 | zh_TW |
dc.description.abstract | The luminescence properties of many gold(I) complexes are sensitive to their molecular arrangements and intermolecular interactions. In general, the aurophilic interactions (AuI… AuI ,ca. 2.5 ~3.8 Å ) of gold(I) complexes strongly affect the emission properties in the solid state. In addition, the aurophilic interaction could be easily regulated by external stimuli, such as mechanical force, volatile organic vapor, heat, and light, thereby making gold(I) complexes an intriguing type of luminescent materials. Our group has been interested in stimuli-responsive materials that contain the rigid H-shaped pentiptycene skeleton. Pentiptycene group has been incorporated into π-conjugated organic or organometallic systems to diminish intermolecular π-stacking and thus improve photoluminescence quantum efficiency in solid state. Moreover, the unique U- and V-cavities created by the two iptycenyl units could lead to different packing modes and supramolecular interactions. Here we report a novel class of pentiptycene-gold(I) hybrid systems bearing different arylacetylene moiety. The phenylacetylene as prototype is named Ph; Complex Naph and An have extended the π-conjugation length, those with substitued at the para position are named OMe, CN and CF3. We study there emission properties with various stimulation and propose a reasonable mechanism through the emission spectrum, single crystal structure and Raman spectroscopy. Our results reveal that all the complexes exhibit emission color change upon treatment of mechanical grinding due to enhanced of aurophilic interactions or the variation of exmeric emission. To our surprise, we found that Ph and its para analouges showed a unique vapochromic luminescent response to the electron-rich aniline vapors, forming red-shifted exciplex emission. As the electron deficiency of the complex increases, the degree of red shift will increase. We conclude that the porous structure is an important factor. In addition, Ph and its para analouges display interesting luminescence response in the crystalline form to UV illumination. Upon photoirradiation, the blue emissive crystals gradually change the emission colors to orangish-red with reduced intensity via a white light emitting intermediate state. It is attributed to photoinduced enhancement of the aurophilic interactions for the tetranuclear cluster that is responsible for the red emission and quenching as a energy trap. | en |
dc.description.provenance | Made available in DSpace on 2021-06-15T12:26:03Z (GMT). No. of bitstreams: 1 U0001-1108202019212400.pdf: 27187418 bytes, checksum: f945abea0a0fe9efca0a04aabacf6031 (MD5) Previous issue date: 2020 | en |
dc.description.tableofcontents | 謝誌 i 摘要 iii Abstract iv 目錄 vi 圖目錄 ix 表目錄 xix 附圖目錄 xx 附表目錄 xxii 第一章 緒論 1 1-1 金(I)錯合物的化學 1 1-1-1 金(I)錯合物的基本結構 1 1-1-2 親金作用力:早期發現 2 1-1-3 親金作用力:定義 5 1-1-4 親金作用力:成因 7 1-1-5 親金作用力:應用 8 1-2 金(I)錯合物的光物理及其應用 12 1-2-1 金(I)錯合物光物理 12 1-2-2 應用於化學感測器 (chemosensors) 16 1-2-3 應用於電致放光 (electroluminescence) 19 1-2-4 應用於細胞顯影 (cell imaging) 21 1-3 金(I)錯合物作為刺激響應材料 23 1-3-1 熱致放光變色 (thermochromic luminescence) 23 1-3-2 力致放光變色 (mechanochromic luminesence) 24 1-3-3 薰致放光變色 (vapochromic luminescence) 28 1-3-4 光致放光變色 (photochromic luminescence) 38 1-4 金(I)-炔基系統 42 1-4-1 金(I)-炔基錯合物的合成 43 1-4-2 金(I)-炔基錯合物的放光性質 44 1-5 含五苯荑基團之固態放光材料 52 1-5-1 苯荑分子的結構特性 52 1-5-2 五苯荑分子的介紹與應用 54 1-6 研究動機 63 第二章 結果與討論 65 2-1 目標錯合物的合成 65 2-2 目標錯合物於溶液態下之光物理 69 2-3 錯合物Ph之聚集態光物理 77 2-4 目標錯合物的晶體結構 79 2-5 目標錯合物之力致放光變色 97 2-6 目標錯合物之薰致放光變色 103 2-7 目標錯合物之光致放光變色 113 2-8 錯合物Ph以拉曼光譜儀觀測其刺激響應性質 122 第三章 結論 128 第四章 實驗部分 129 4-1 實驗藥品及溶劑 129 4-2 實驗步驟 132 力致放光變色實驗 132 薰致放光變色實驗 132 光致放光變色實驗 132 4-3實驗儀器 133 4-3 合成步驟 138 化合物39之合成 138 化合物40之合成 139 化合物41之合成 139 化合物42之合成 140 化合物Pi之合成 141 二甲硫醚氯化亞金(I)之合成 142 化合物43a~43c之合成 142 化合物44a~44c之合成 143 化合物45a~45c之合成 144 化合物46a之合成 144 化合物46b之合成 145 化合物47b~47c之合成 146 化合物48a~48c之合成 146 化合物48c另一合成方法 147 錯合物Ph之合成 147 錯合物Naph之合成 148 錯合物An之合成 149 錯合物CN之合成 150 錯合物OMe之合成 151 錯合物CF3之合成 152 參考資料 152 附圖 160 | |
dc.language.iso | zh-TW | |
dc.title | 含五苯荑金(I)炔基錯合物之刺激響應放光性質之研究 | zh_TW |
dc.title | Stimuli-Responsive Photoluminescent Properties of Pentiptycene-Containing Gold(I) Acetylide Complexes | en |
dc.type | Thesis | |
dc.date.schoolyear | 108-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 彭旭明(Shie-Ming Peng),鄭原忠(Yuan-Chung Cheng),江建文(Kien Voon Kong) | |
dc.subject.keyword | 金(I)-炔基錯合物,親金作用力,力致放光變色,薰致放光變色,光致放光變色,激發複合體,孔洞型晶體結構, | zh_TW |
dc.subject.keyword | Gold(I) Acetylide complex,Aurophilic interactions,Mechanochromic Luminescence,Vapochromic Luminescence,Photoochromic Luminescence,Exciplex,Porous Crystal Structures, | en |
dc.relation.page | 296 | |
dc.identifier.doi | 10.6342/NTU202003002 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2020-08-18 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
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