臺灣博碩士論文加值系統

　　本研究於2019年6月及8月以拖網方式採集台灣西南沿海36個測站表層海水之微塑膠(Microplastics, MPs)樣品。採集之表層海水樣品經篩選、浮選、消化及過濾後。以顯微鏡觀察及拍照濾膜上之MPs，並統計表層海水中MPs之豐度、大小、形狀及顏色等基本性質。另外使用傅立葉轉換紅外線儀(Fourier-transform infrared spectroscopy, FTIR)進一步鑑定材質。MPs上的多環芳香烴化合物(Polycyclic aromatic hydrocarbons, PAHs)、鄰苯二甲酸酯類(Phthalates, PAEs)、壬基酚(Nonyl phenol, NP)及辛基苯酚(Octyl phenol, OP)是經有機溶劑萃取及濃縮後，以氣相層析/質譜儀(GC/MS)進行定性定量分析，來了解MPs樣品等化合物之濃度。研究目的為: (1)瞭解西南沿海表層海水中MPs的豐度、大小、形狀、顏色及種類的時空分佈；(2)評估MPs可能的主要來源；(3) MPs的PAHs、PAEs、NP、OP濃度、組成及可能來源。
　　研究結果顯示，所有測站皆有發現MPs，僅有8月1個測站未發現MPs，顯示MPs普遍分佈於沿海區域，豐度介於0.06–1.47 item/m3，其中約30%的MPs來自於河口區，顯示MPs主要是由陸源輸入。8月MPs豐度(0.36±0.31 item/m3)較6月(0.24±0.16 item/m3)來得高，可能受降雨之影響。MPs大小最多介於1–2 mm之尺寸，約佔所有MPs的40%，0.33–1 mm (19.1%)為次之。歸類五種不同形狀的MPs，包括了柔珠(pellet)、薄膜(film)、發泡(foam)、線狀(line)、碎塊(fragment)，碎塊為最常見的形狀，佔總MPs的82%。有色塑膠佔最高比例(58%)，其次為白色(17%)及透明(28%)。MPs的材質，以聚乙烯(Polyethylene, PE) (67%)及聚丙烯(Polypropylene, PP) (27%)佔最多，而聚苯乙烯(Polystyrene, PS)及聚氯乙烯(Polyvinyl Chloride, PVC)比例皆小於4%。綜合形狀、顏色、材質結果，推測MPs主要來自大型塑膠分解的二次來源，而柔珠等一次來源僅佔一小部分。
　　MPs上的總PAHs濃度範圍介於67–3595 μg/kg dw，MPs上吸附的PAHs以3環(56%)為主，且以化合物菲(Phenanthrene, PH)佔37%為最高。利用Anthracene/(Anthracene+PH)和Fluoranthene/(Fluoranthene+ Pyrene)特徵比值分析結果顯示，MPs吸附的PAHs來源為石油、燃燒及石油與燃燒的混合來源，MPs吸附的PAHs相當複雜，顯示MPs吸附的PAHs並不為單一來源。MPs測得的PAEs濃度範圍介於3.7–174 mg/kg dw，主要以高分子量的PAEs(94.3%)為主，且由鄰苯二甲酸二(2-乙基己基)酯(DEHP) (59%)佔最多。OP的濃度範圍介於16–557 μg/kg dw，NP的濃度範圍介於54–2836 μg/kg dw，結果顯示，台灣西南沿海MPs中吸附多種內分泌干擾及持久性有機物質，增加被生物誤食的不利風險。

In this study, samples of microplastics (MPs) from the surface seawater of 36 stations on the southwest coast of Taiwan were collected by trawling in June and August 2019. The collected surface seawater samples are screened, floated, digested and filtered. Observe and photograph the MPs on the filter membrane with a microscope, and assess the basic properties such as the abundance, size, shape and color of MPs in the surface seawater. In addition, Fourier-transform infrared spectroscopy (FTIR) was used to further identify the MPs type. Polycyclic aromatic hydrocarbons (PAHs), phthalates (PAEs), 4-nonyl phenol (NP) and 4-tert-octyl phenol (OP) on MPs are using organic solvent extraction and concentration, qualitative and quantitative analysis is performed by gas chromatography/mass spectrometry (GC/MS) to understand the concentration of compounds such as MPs samples. The research objectives are: (1) To understand the spatial and temporal distribution of MPs abundance, size, shape, color, and species in the surface seawater of the southwestern coastal waters; (2) To assess the possible main sources of MPs; (3)PAHs, PAEs, NP, OP concentrations, compositions in MPs and possible sources.
the results showed that MPs were found at all stations. Only one station in August did not find MPs, MPs abundance range from 0.06–1.47 item/m3 showing that MPs are generally distributed in coast area, about 30% abundance from river mouth, it was shown that MPs were mainly imported from land sources. The abundance of MPs in August (0.36±0.31 item/m3) is higher than that in June (0.24±0.16 item/m3), which may be affected by rainfall. The proportion of MPs between 1–2 mm is the highest with 40%, followed by 0.33–1 mm (19.1%). MPs are classified into five different shapes, including pellet, film, foam, line, and fragment. Fragment is the most common shape, accounting for the 82% of total MPs. Colored plastic accounted for the highest proportion (58%), white (17%) and transparent (28%) were the second highest. MPs most type is polyethylene (PE) (67%) and polypropylene (PP) (27%), while polystyrene (PS) and Polyvinyl Chloride (PVC) the proportion is less than 4%. Based on the results of shape, color, and type, it is speculated that MPs mainly come from secondary sources of large-scale plastic decomposition, while primary sources such as soft beads only account for a small part.
The concentration of total PAHs on MPs range is 67–3595 μg/kg dw. The PAHs adsorbed on MPs were dominated by 3 rings (56%), with the compound Phenanthrene (PH) accounting for 37%. The analysis results of Anthracene/(Anthracene+PH) and Fluoranthene/(Fluoranthene+Pyrene) characteristic ratio show that the source of PAHs adsorbed by MPs is petroleum, combustion and mixed sources of oil and combustion. The PAHs adsorbed by MPs are complex, showing the PAHs adsorbed by MPs is not from a single source. The concentration of PAEs measured by MPs range is from 3.7–174 mg/kg dw, mainly composed of high molecular weight PAEs (94.3%), and consisted of bis(2-ethylhexyl) phthalate (DEHP) (59 %) accounted for the most. The concentration of OP range is 16–557 μg/kg dw, and the concentration of NP range is 54–2836 μg/kg dw. The results show that endocrine interference and persistent organic substances are adsorbed in MPs on the southwestern coast of Taiwan, it will increasing the biologcal ingestion hazard.

目錄
摘要 iii
Abstract v
目錄 vii
圖目錄 xi
表目錄 xiii
第一章 前言 1
1.1研究動機 1
1.2研究目的 2
第二章 文獻回顧 3
2.1研究區域 3
2.2 微塑膠 4
2.2.1微塑膠特性 4
2.2.2微塑膠的生物危害 4
2.2.3微塑膠主要來源與現況 5
2.2.4微塑膠的化學吸附 7
2.3 多環芳香烴化合物 9
2.3.1 多環芳香烴物化特性 9
2.3.2 多環芳香烴來源 10
2.3.3多環芳香烴危害 11
2.3.4多環芳香烴來源評估 16
2.4 鄰苯二甲酸酯類 18
2.4.1 鄰苯二甲酸酯類來源 18
2.4.2鄰苯二甲酸酯的危害 19
2.5辛基酚及壬基酚 20
2.5.1壬基酚及辛基酚的來源 20
2.5.2壬基酚及辛基酚的危害 21
第三章 研究材料與方法 22
3.1 研究架構 22
3.2 採樣地點及採樣規劃 24
3.3 實驗藥品及試劑 28
3.4 微塑膠樣品鑑定 32
3.5 微塑膠尺寸測量 33
3.6 樣品分析 34
第四章 品保品管 36
4.1 GC/MS例行性校正 36
4.2 GC/MS分析苯環類化合物的設置條件 37
4.3 空白試驗 41
4.4 檢量線 42
4.5 偵測極限 45
第五章 結果與討論 47
5.1 微塑膠豐度及分佈 47
5.2 微塑膠粒徑、形狀、顏色 54
5.3 微塑膠種類 62
5.4 微塑膠吸附的多環芳香烴濃度、環數及化合物分布 67
5.5 微塑膠PAHs特徵比值分析 80
5.6 微塑膠上的鄰苯二甲酸酯、壬基酚、辛基苯酚 83
第六章 結論與未來工作 92
6.1 結論 92
6.2 建議 94
參考文獻 95
附錄一 124
附錄二 161
附錄三 207

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