臺灣博碩士論文加值系統

本研究主題為將天然資源將轉化成為光電材料，分為三個部分：第一部分為將天然廢棄物(貝殼)轉化成白光螢光粉；第二部分是以矽藻的葉綠素萃取物作為矽太陽能電池的抗反射層；第三部分是使用矽藻殼結合GaN或Rh6G等增益介質演示隨機激光現象。
第一個研究是利用一般的固態反應法製備單相磷酸釓鈣(Ca9Gd(PO4)7, CGP)共摻雜銪二價陽離子(Eu2+)與錳二價陽離子(Mn2+)的白光螢光粉(CGP:Eu2+,Mn2+)，其中鈣的來源是由天然的生物貝殼(文蛤)所轉化而來。我們以X光粉末繞射(X-ray powder diffraction, XRD)、光激發螢光激發光譜(photoluminescence excitation, PLE)與光激發螢光光譜(photoluminescence, PL)做螢光粉的定性分析。由以波長為350 nm的光源激發螢光粉所得之放光光譜，可觀察到一個375到650 nm的寬放光帶，又由以波長490 nm光源所激發的光譜，可以觀察到250-450 nm的寬廣激發帶。以上的結果說明Eu2+可以有效地吸收近紫外光(300-400 nm)，且發出藍光到紅光之間的寬帶放光，因此Eu2+可以做為感光體(sensitizer)，轉移部份能量到Mn2+活化體(activater)。我們將白光CGP:Eu2+,Mn2+螢光粉與紫外光發光二極體結合，成功製作出白光發光二極體。
第二部分的研究是利用酒精溶劑從矽藻萃取葉綠素，這種萃取方式比使用其他溶劑(如丙酮、己烷)的作法更為安全與環保。葉綠素萃取物的光學性質是以PL與紫外光-可見光吸收光譜(UV-vis spectrophotometer)做分析，在PL的放光光譜中，我們沒有發現葉綠素c的波峰，這可能是因為其放光強度較弱或者是在萃取物中所含的比例遠低於葉綠素a，因此，矽藻萃取物的PL放光來自葉綠素a的成分，經由光譜分析得到葉綠素a濃度約100 mg L-1，葉綠素a可吸收紫外光到藍光(250-470 nm)並發出紅光(670 nm)。由上述的光學分析，矽藻萃取物中光子能量轉換的主要活性成分是葉綠素a，矽藻萃取物可以做為紫外到紅光光子轉換的材料。我們將矽藻萃取物做為抗反射層與光子能量轉換層，做為提升矽太陽能電池效率的方法。
在最後的部分，我們展示一種由生物性矽藻殼組成的複合材料在紫外和可見光區的產生隨機雷射現象，由於矽藻結構的多孔網絡具有低的光損耗，我們以生物矽藻結構做為散射中心，使GaN 薄膜和Rh6G 染料的光激發螢光產生隨機雷射現象。有趣的是，透過矽藻結構，可以容易地獲得具有非常尖銳波峰的紫外和可見光範圍隨機激光現象，結果顯示矽藻殼的尺寸大小可以形成產生隨機雷射的光學共振條件。

We have investigated on the converting natural resources into the optoelectronic materials. The research topics include: (1) Converting natural waste (shell) into the white-light phosphors. (2) Using chlorophyll extract from diatom algae as a anti-reflection layer on silicon solar cells. (3) Using GaN or Rh6G as gain media to couple with diatom frustules for the demonstration of random laser action.
The first topic is the preparation of co-doping Eu2+, Mn2+ into a single-phased Ca9Gd(PO4)7 (CGP) white-light phosphors by conventional solid state reaction method. The sources of calcium which hosted in CGP:Eu2+,Mn2+ were transferred by biological shellfish (clams). The X-ray powder diffraction (XRD), photoluminescence excitation (PLE) and photoluminescence (PL) spectra were used to ensure the physical properties of CGP:Eu2+,Mn2+. The PL spectra by 350 nm excitation showed a broad blue-greenish emission band ranging from 375 nm to 650 nm, and the PLE spectra (λem = 490 nm) showed a broad hump from 250 to 450 nm. As the above results showed the Eu2+ could efficiently absorb near ultraviolet (300–400 nm) light and give blue to red broadband emissions. Therefore, Eu2+ can act as a sensitizer, transferring a part of its energy to activator ions, manganese ions (Mn2+). Finally, we successfully demonstrated the fabrication and packaging of a phosphor-converted white light-emitting diodes (pc-WLEDs) by pumping a white-emitting CGP: Eu2+, Mn2+ phosphor with an UV LED chip.
For the second topic, chlorophyll (chl) was extracted from diatom with ethanol. Comparing with other solvents (such as actone and hexane), the use of ethanol was more safety and environmentally friendly. The spectra of chlorophyll extraction were well characterized by UV-vis spectrophotometer and PL techniques. In our measurements, we detected no PL emission for chlorophyll c (chl-c), which is likely due to its relatively weaker natural emission or much lower fraction in the sample as compared with chlorophyll a (chl-a). Thus, the monitored PL peak for the diatom extract can be attributed to chl-a content, which is determined spectroscopically to be about 100 mg L-1. Chl-a absorted the UV to blue (250–470 nm) light, than emitted red light (670 nm). From the above optical analysis, the primary active content (chl-a) is responsible for photon energy conversion in the diatom extract, which makes the diatom extract be an attractive candidate for violet-to-red photon conversion. We will demonstrated an approach to improve the Efficiency of silicon solar cells by incorporating the diatom extract as an layers of antireflection of light and photon energy conversion.
Finally, we demonstrated a random laser actions in ultraviolet and visible regions based on the composites consisting of bio-derived diatom frustules. Owing to the low optical loss from porous network of diatom structures, the random laser actions were generated from GaN film or Rh6G dye via using biological diatoms as scattering centers. Interestingly, both ultraviolet and visible-range random laser actions with very sharp peaks can be easily obtained, indicating the size of diatom frustules can constitute the optical resonance conditions for generating random lasers.

謝誌 I
摘要 III
Abstract V
目錄 VII
圖目錄 XII
表目錄 XVI
第一章 緒論 1
1-1 前言 1
1-2 研究動機與目的 3
第二章 背景介紹 5
2-1螢光粉 5
2-1-1 螢光粉應具備的條件 5
2-1-2光的特性參數 6
2-1-3 白光發光二極體(WLED) 8
2-1-4 單相白光螢光粉 8
2-1-5 能量轉移機制 10
2-1-6 螢光粉的主體材料 12
2-1-6-1 磷酸鈣(β-Ca3(PO4)2, β-TCP) 12
2-1-6-2 磷酸釔鈣(Ca9Y(PO4)7, CYP) 12
2-1-6-3 矽酸磷酸鈣(Ca14.92(PO4)2.35(SiO4)5.65, CPS) 12
2-1-6-4 磷酸釓鈣(Ca9Gd(PO4)7, CGP)主體材料 12
2-1-7 螢光粉活化體之光學特性 13
2-1-7-1 銪三價陽離子(Eu3+) 13
2-1-7-2 銪二價陽離子(Eu2+) 14
2-1-7-1 鏑三價陽離子(Dy3+) 14
2-1-8 以活性碳建構的還原環境 15
2-2 貝殼廢棄物 16
2-2-1 貝殼的組成與結構 16
2-2-2 貝殼廢棄物(文蛤)之總量 17
2-2-3 貝殼結構的相轉變與應用 17
2-3 葉綠素的光電應用 18
2-3-1 葉綠素的萃取與定量 18
2-3-2 矽太陽能電池 18
2-4 矽藻殼的光電應用 19
2-4-1 隨機雷射 19
2-4-2 仿生與隨機雷射 20
第三章以貝殼為基礎轉化成螢光粉材料 21
3-1 貝殼結構相轉換：天然源碳酸鈣 21
3-1-1 實驗提要 21
3-1-2 實驗部分 21
3-1-2-1 實驗藥品 21
3-1-2-2 實驗步驟 21
3-1-2-3 分析儀器 21
3-1-3 結果與討論 22
3-1-3-1 文蛤殼結構之相轉換 22
3-1-3-2 文蛤殼結構之雜質分析 22
3-1-3-3 文蛤殼轉化為天然源碳酸鈣之成本估算 23
3-1-4 結論 26
3-2 以文蛤殼為基礎的[主體 + 活化體]螢光粉製備 27
3-2-1 實驗提要 27
3-2-2 實驗部分 27
3-2-2-1 實驗藥品 27
3-2-2-2 樣品合成步驟 28
3-2-2-3 實驗儀器 28
3-2-3 結果與討論 29
3-2-3-1以文蛤殼為基礎的[主體 + 活化體]螢光粉之結構分析 29
3-2-3-2以文蛤殼為基礎的[主體 + 活化體]螢光粉之光激發螢光分析 29
3-2-4 結論 32
3-3以文蛤殼為基礎的[主體 + 活化體 + 感光體]白光螢光粉製備 33
3-3-1 實驗提要 33
3-3-2 實驗部分 33
3-3-2-1 實驗藥品 33
3-3-2-2 樣品合成步驟 34
3-3-2-3 實驗儀器 34
3-3-3 結果與討論 35
3-3-3-1以文蛤殼為基礎的[主體 + 活化體 + 感光體]白光螢光粉之結構分析與表徵觀察 35
3-3-3-2 以文蛤殼為基礎的[主體 + 活化體 + 感光體]白光螢光粉之光學特性 35
3-3-4 結論 48
3-4其他以文蛤殼為基礎的螢光粉 49
3-4-1 以文蛤殼為基礎的CGP:Eu3+螢光粉 49
3-4-2 以文蛤殼為基礎的β-TCP:Dy3+螢光粉 49
3-4-3 以文蛤殼為基礎的CYP:Dy3+螢光粉 50
3-4-4 以文蛤殼與矽藻土為基礎CPS:Eu3+螢光粉 50
3-4-5 結論 55
第四章 矽藻的太陽能應用與矽藻殼的雷射應用 56
4-1 矽藻葉綠素之萃取與其太陽能元件應用 56
4-1-1 實驗提要 56
4-1-2 實驗部分 56
4-1-2-1 矽藻培養 56
4-1-2-2 實驗藥品 56
4-1-2-3 實驗方法 57
4-1-2-3.1 矽藻萃取葉綠素的方法 57
4-1-2-3.2 葉綠素A的定量分析 58
4-1-2-3.3 葉綠素應用於太陽能電池 58
5-1-2-4 實驗儀器 58
4-1-3 結果與討論 59
4-1-3-1 矽藻萃取物中葉綠素a之定量 59
4-1-3-1.1 以分光光度計分析 59
4-1-3-1.2 以光激發光譜儀分析 59
4-1-3-2 矽藻萃取葉綠素於太陽能電池應用成果[109] 65
4-1-4 結論 66
4-2 矽藻殼的隨機雷射應用 67
4-2-1 實驗提要 67
4-2-2 實驗部分 67
4-2-2-1 實驗藥品 67
4-2-2-2 實驗方法 67
4-2-2-3 實驗儀器 67
4-2-3 結果與討論 67
4-2-3-1 矽藻土之表面特徵與型貌 67
4-2-3-2矽藻殼應用於隨機雷射成果[113] 68
4-2-4 結論 69
總結 70
歷年發表著作一覽 71
SCI 71
代表著作 71
參考著作 71
國際研討會 72
2012 SPIE Photonics Asia - Beijing, China. 72
2015 Global Engineering & Applied Science Conference - Tokyo, Japan. 72
國內研討會 73
中華民國燃燒學會第二十二屆學術研討會 73
專利 73
參考文獻 74
 

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