臺灣博碩士論文加值系統

近數十年來，奈米材料被廣泛應用於各種科學領域上及日常生活用品中，其極有可能因直接/間接方式流佈於水體環境中，危害生態環境及人體健康，為了瞭解奈米微粒於水體環境中之行為及反應，本研究乃利用自行製備之奈米微粒(Nano-ZnO、Nano-Ag及Nano-CeO2)添加於不同水體介質之中，針對不同之環境因子、水質參數及水中常見物質探討奈米微粒於不同水體環境中可能之轉化及宿命。
本研究發現，奈米微粒於水中之溶解度會受pH影響，當pH=3時，奈米微粒有最大溶解度，Nano-ZnO之溶解度可達100%，而Nano-Ag及Nano-CeO2之溶解度則低於2%；至於一般環境之溫度，則對其溶解度之影響較小。pH值及離子強度會影響奈米微粒在水環境中之穩定性，奈米微粒於水環境中之負界達電位隨pH值上升而增大，顯示其懸浮分散性越佳；水中之離子強度大，則會壓縮奈米微粒之電雙層結構，使奈米微粒團聚，當離子強度越大時，其團聚現象越為明顯，故添加電荷價數越高之電解質，則奈米微粒團聚效應越為明顯，當離子強度高於臨界聚集濃度時，奈米微粒之聚集效率(α)則趨於穩定，此現象於自然水體組別中也可觀察到。研究結果顯示，Nano-ZnO於pH=10之水體環境中，其Zn2+可與OH-結合形成Zn(OH)2，此可由X-光繞射之特性坡峰加以確認；同樣地，Nano-CeO2於水中會釋出Ce4+，並與水環境中之SO42-結合形成Ce(SO4)2之新結晶相，上述結果顯示奈米微粒可能會與水環境介質中之溶解性陰陽離子反應並生成不同物質。此外，水環境中常見之腐植酸則有助於奈米微粒之懸浮穩定性，使其於較長時間內仍維持一定尺寸。然而當鄰苯二甲酸二(2-乙基己基)酯、紅黴素與奈米微粒同時存在於水環境中，奈米微粒對上述新興污染物之影響並不明顯。於模擬現實環境之組別中，水中之Nano-ZnO因陽光照射使其具有光催化之作用，導致具有殺菌功能；至於Nano-Ag，於自然水體中即有極強之抗菌能力，能在一小時內使水體中之總菌生存率降低至2%以下。
綜合而言，本研究發現奈米微粒於水環境介質中其穩定性易受環境因子、水質參數及水中物質之影響，其可能與水環境中之溶解性陰陽離子結合形成新結晶相，或因聚集而沉降，或因其特性而具殺菌功能。

The fate and transformation of laboratory-prepared nano-ZnO, nano-Ag and nano-CeO2 in three aqueous solutions under different environmental conditions were investigated in this work. Over the past decades nanomaterials have been widely used in different technical fields and consumer goods. As a result, nanomaterials might enter the environmental media via different routes and then posed potential hazards to the environment and human health. Researches in this regard have received much attention worldwide. In this work it was found that the solubility of each nanomaterial was highly influenced by the solution pH, but not by the solution temperature. The maximal solubility for the tested nanomaterials was obtained at pH 3, namely about 100% for nano-ZnO and lower than 2% for both nano-Ag and nano-CeO2. The solution pH and ionic strength were found to affect the stability of nanoparticles in different aquatic environments. For the solution pH of higher than the isoelectric point of the concerned nanomaterial, the higher the solution pH is, the greater the degree of stabilization of nanoparticles would be. On the contrary, nanoparticles aggregated as the ionic strength of the solution exceeded its critical aggregation concentration (CAC). CAC for each concerned nanomaterial could also be graphically determined as the attachment efficiency (α) of nanoparticles increased with increasing ionic strength of the solution and then leveled off after reaching CAC. Experimental results also showed that Zn(OH)2(s) would form when nano-ZnO was in the solution of pH 10. The crystalline structure of the said precipitates was confirmed by X-ray diffraction. Likewise, Ce4+ dissolved from nano-CeO2 reacted with SO42- in aqueous solution yielding Ce(SO4)2(s). Clearly, transformation of nanomaterials might take place when they are in contact with various species in different aquatic environments. Humic acid in aqueous solution was found to be beneficial to the stability of nanomaterial of concern. Efforts have also been made to study the reaction behaviors among di(2-ethylhexyl)phthalate, erythromycin, and selected nanomaterials when they co-existed in the same solution. Their interactions, however, seemed to be unobvious. In this work it was found that under sunlight irradiation nano-ZnO did show its antibiotic effect due to photocatalysis. Nano-Ag was proven to have a strong antibacterial ability even in natural aquatic environments. It yielded the total bacteria survival ratio of less than 2% within one hour of reaction. In summary, the findings of this study showed that the behaviors of nano-ZnO, nano-Ag, and nano-CeO2 in aqueous solutions could be greatly influenced by different factors in different reaction systems.

聲明切結書 i
謝誌 ii
摘要 iii
Abstract v
目錄 vii
圖目錄 xii
表目錄 xvii
照片目錄 xviii
第一章 前言 1
1-1研究緣起 1
1-2研究目的 2
1-3研究內容與架構 2
第二章 文獻回顧 5
2-1奈米材料之簡介 5
2-1-1無機奈米材料 6
2-1-1-1奈米級氧化鋅之特性與應用 6
2-1-1-2奈米銀之特性與應用 8
2-1-1-3奈米級二氧化鈰之特性與應用 9
2-2奈米微粒間之作用力 10
2-2-1 DLVO理論 10
2-2-2奈米級氧化鋅於水介質中之穩定性 12
2-2-3奈米銀於水介質中之穩定性 15
2-2-4奈米級二氧化鈰於水介質中之穩定性 18
2-3環境荷爾蒙及藥物 19
2-3-1鄰苯二甲酸二(2-乙基己基)酯 21
2-3-2紅黴素 23
第三章 實驗材料、設備與方法 24
3-1實驗材料與試劑 24
3-1-1水樣來源 24
3-1-2 材料與試劑 24
3-2實驗設備 27
3-3實驗方法 30
3-3-1奈米微粒製備 30
3-3-1-1奈米級ZnO製備 30
3-3-1-2奈米級Ag製備 30
3-3-1-3奈米級CeO2製備 31
3-3-2奈米微粒之基本特性分析 31
3-3-2-1晶型鑑定 31
3-3-2-2微粒型態及其元素分析 31
3-3-2-3等電點分析 32
3-3-3水樣分析方法 33
3-3-3-1基本水質分析 33
3-3-1-2含DEHP及紅黴素之水樣前處理程序 34
3-3-4奈米微粒於水環境介質中溶解反應探討 35
3-3-5奈米微粒於水環境介質中之團聚與分散性探討 35
3-3-5-1不同pH與溫度對奈米微粒於水環境介質中之團聚與分散性探討 35
3-3-5-2離子強度對奈米微粒於水環境介質中之團聚與分散性影響探討 36
3-3-6奈米微粒與水環境介質中溶解性物種之反應探討 37
3-3-7奈米微粒與水環境介質中膠體粒子之反應探討 38
3-3-8奈米微粒與水環境介質中微生物之反應探討 38
3-3-9奈米微粒與水環境介質中新興污染物之反應探討 39
第四章 結果與討論 40
4-1奈米微粒基本性質分析 40
4-1-1 X-光繞射儀(X-Ray Diffraction, XRD)之分析 40
4-1-2環境掃描式電子顯微鏡-能量分散光譜儀(ESEM-EDS) 43
4-1-3穿透式電子顯微鏡(TEM)之分析 45
4-1-4等電點分析 47
4-2水樣基本性質分析 49
4-3奈米微粒於水環境介質中溶解反應探討 51
4-3-1溫度及pH值對Nano-ZnO於水介質中溶解性探討 51
4-3-2溫度及pH值對Nano-Ag於水介質中溶解性探討 53
4-3-3溫度及pH值對Nano-CeO2於水介質中溶解性探討 56
4-4奈米微粒於水環境介質中之穩定性探討 58
4-4-1溫度及pH值對Nano-ZnO於水介質之穩定性影響 58
4-4-2溫度及pH值對Nano-Ag於水介質之穩定性影響 60
4-4-3溫度及pH值對Nano-CeO2於水介質之穩定性影響 62
4-4-4離子強度對Nano-ZnO於水介質之穩定性影響 64
4-4-5離子強度對Nano-Ag於水介質之穩定性影響 67
4-4-6離子強度對Nano-CeO2於水介質之穩定性影響 69
4-5奈米微粒與水環境介質中溶解性物種之反應探討 72
4-5-1陰陽離子對Nano-ZnO於水介質之物化特性影響 72
4-5-2陰陽離子對Nano-Ag於水介質之物化特性影響 76
4-5-3陰陽離子對Nano-CeO2於水介質之物化特性影響 79
4-6奈米微粒與水環境介質中膠體粒子之反應探討 81
4-6-1 Nano-ZnO與水環境介質中腐植酸之反應探討 81
4-6-2 Nano-Ag與水環境介質中腐植酸之反應探討 86
4-6-3 Nano-CeO2與水環境介質中腐植酸之反應探討 90
4-6-4 Nano-ZnO與水環境介質中二氧化錳之反應探討 94
4-6-5 Nano-Ag與水環境介質中二氧化錳之反應探討 98
4-6-6 Nano-CeO2與水環境介質中二氧化錳之反應探討 102
4-7奈米微粒與水環境介質中微生物之反應探討 106
4-7-1周遭無菌環境下之水體中其總菌落數變化 106
4-7-2室外現實環境下之水體中其總菌落數變化 109
4-8奈米微粒與水環境介質中污染物質之反應探討 112
4-8-1奈米微粒與水環境介質中DEHP之反應探討 112
4-8-2奈米微粒與水環境介質中紅黴素之反應探討 115
第五章 結論與建議 117
5-1結論 117
5-2建議 119
參考文獻 120
碩士在學期間發表之學術論文 135

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