以二氧化錳去除水中多重藥物之研究

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Title:	以二氧化錳去除水中多重藥物之研究 Removal of Multiple Pharmaceuticals in water by Manganese Dioxide
Authors:	鄧祥寧 Teng, Hsiang-ning
Contributors:	胡景堯
Keywords:	乙醯胺酚;雙氯芬酸;磺胺甲噁唑;二氧化錳;化學分析影像能譜儀;高效液相層析儀;極致液相層析-四極桿飛行時間質譜儀 Acetaminophen;Diclofenac;Sulfamethoxazole;β-MnO2;ESCA;HPLC;UPLC-Q-TOF-MS
Date:	2014-07-10
Issue Date:	2019-09-02 10:53:33 (UTC+8)
Abstract:	隨著現代醫學發展與進步，人類用藥逐漸多元化，在廢水系統及表水系統皆有偵測到濃度範圍在ng/L~μg/L之人類用藥。相關研究指出，一些藥物長期接觸後可能會對人體或動植物有危害。二氧化錳(MnO2)存在於土壤與底泥中，為自然界重要的氧化劑之一，具有良好的氧化還原能力，能有效降解有機污染物，其具有高的還原電位，對於酚(Phenol)、氯酚(Chlorophenol)、苯胺(Anilines)、及磷酸類(Phosphonate)化合物有良好的分解效果。先前關於二氧化錳去除藥物之研究多只針對一種藥物，但廢水中通常存在多種藥物。因此在多重藥物系統中，應有系統性的調查藥物在二氧化錳上的吸附及氧化之競爭情形。本研究選用三種不同類型、廣泛被人類使用、且經常在表廢水系統中偵測到之藥物，分別為乙醯胺酚、雙氯芬酸、及磺胺甲噁唑探討多重藥物在二氧化錳表面的吸附氧化情形，並且調查二氧化錳劑量、酸鹼值、及溫度的影響。實驗結果發現，環境酸鹼值會顯著影響藥物去除率，三種藥物皆是酸性為去除之最佳條件，而乙醯胺酚在鹼性去除效果優於中性，在雙氯芬酸及磺胺甲噁唑則是中性的去除效果優於鹼性，觀察到與先前研究有相似的結果。而二氧化錳的劑量增加以及溫度提高也會增加藥物之去除率。化學分析影像能譜儀(ESCA)結果顯示，當酸鹼值增加，則二氧化錳表面二價錳之比例也隨著上升。副產物定性部份，使用UPLC-Q-TOF-MS鑑定其副產物，發現到酸性環境下，雙氯芬酸有一個副產物，鹼性條件下，會產生乙醯胺酚之二聚體及三聚體，此研究有助於進一步了解藥物在自然環境中的宿命。 With the development and progress of modern medicine, human pharma- ceuticals has become more diversity. In surface water and wastewater system, many pharmaceuticals have been frequently detected, and their concentrations usually range from ng/L to μg/L. Some studies indicated that human exposure to drugs in long term, it may be hazardous to human or animal or plants. Manganese oxides/hydroxides are among the most important naturally occurring oxidants in facilitating organic pollutant transformation in soils and sediments and deserve particular attention due to their high reduction potentials. It is an effective oxidant for a wide range of pollutants including phenols, chlorophenols, anilines, and phosphates. A lot of researches have been done about the removal characteristics of the single pharmaceutical compound by manganese oxides. The wastewater, however, usually contains various pharmaceuticals. The effects of competitive adsorption and oxidation by manganese oxides need to be systematically investigated in mixed pharmaceuticals system. This study chose three different types of drugs which are frequently used by human and often be detected in surface water and wastewater system ---acetaminophen, diclofenac, and Sulfamethoxazole to investigate their adsorption and oxidation on the manganese oxide surface. The effects of dose of manganese oxides, pH and temperature were investigated. The results indicate that pH significantly influenced the removal of pharmaceuticals. The best removal of the three pharmaceuticals appeared in acidic condition. The removal of acetaminophen in alkali condition was better than in neutral. While the removal of diclofenac and sulfamethoxazole in neutral condition was better than alkali condition. Similar phenomenon has been observed in previous studies. Increasing the dosage of manganese dioxide and raising the temperature increased the removal of drugs. The results of Electron Spectroscopy for Chemical Analysis (ESCA) revealed that as pH increasing, the Mn(II) proportion increase in the β-MnO2 particle surface. HPLC-DAD and TOF–MS was used to identify oxidation products. In acidic environment, diclofenac has a byproduct. In basic condition, we find dimer and timer products of acetaminophen. These results are useful in understanding the fate of pharmaceuticals in natural systems.
Description:	碩士指導教授-胡景堯委員-官文惠委員-闕蓓德
Data Type:	thesis
Appears in Collections:	[School of Public Health] Dissertations/Theses

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