臺灣博碩士論文加值系統

本研究於108年1、4及7月採集高雄港的港口(2測站)、南航道(6測站)、北航道(8測站)及河口(4測站)區域，共60個表層沉積物樣品。沉積物物化特性之分析包括：粒徑分佈、總有機碳(Total organic carbon, TOC)、pH、氧化還原電位、酸揮發性硫化物(Acid-volatile sulfides, AVS)及金屬(銅、鉛、鎳、鎘、鋅、鉻、錳、鐵)等。其中，金屬分別以總量(Total metal, TM)消化、AVS同步萃取金屬(Simultaneously extracted metals, SEM)與序列萃取法(Sequential extraction procedures, SEP)三種方式進行分析。金屬分析結果進一步以污染負荷指數(Pollution load index, PLI)、毒性風險指數(Toxic risk index, TRI)、酸揮發硫化物的沉積物平衡分配基準(Equilibrium partitioning sediment benchmarks with AVS and TOC, ESBAVS OC)、金屬生物可利用指數(bioavailability index of metals, BI)及金屬潛在移動性指數(Potential mobility index of metals, PMI)評估港區沉積物中金屬的潛在風險、潛在移動性及生物可利用性。此外，利用生物毒性法(Microtox)進行沉積物毒性測試，並與三種金屬化學方法之評估結果比較，藉以綜合評估港區沉積物金屬之潛在毒性。
高雄港沉積物中金屬總量濃度為：銅8.57–858 mg/kg；鉛10.2–90.8 mg/kg；鎳20.1–79.0 mg/kg；鎘0.01–1.98 mg/kg；鋅69.2–1367 mg/kg；鉻17.1–249 mg/kg；錳100–956 mg/kg。港區沉積物中金屬總量在空間分布上呈現河口> 航道> 港口，顯示港區沉積物中金屬主要來自上游河川注入之廢污水。以金屬總量為基礎的沉積物評估指標(PLI及TRI)結果顯示，河口及航道沉積物受到大量金屬污染，具有低至極高的金屬毒性風險。而港口沉積物受到金屬污染程度小，其毒性風險低。由AVS同步萃取金屬分析結果發現，SEM分布情形與總量類似，並佔金屬總量75 %以上。但沉積物進一步以平衡分配基準指標(ESBAVS OC)評估，發現河口沉積物富含AVS (15.3–172 μmol/g)及TOC (1.12–7.69 %)，由於二價金屬會與AVS結合形成較不溶金屬硫化物，即使河口沉積物金屬污染嚴重，但其生物可利用性低。而部分航道及港口沉積物中金屬污染程度低，但AVS及TOC含量亦較少，其沉積物中金屬的生物可利用性反而較河口沉積物高。根據SEP的評估指標(BI及PMI)發現，部分南航道及鹽水港溪沉積物中金屬具有潛在的移動性，但整體而言，港區沉積物中金屬的生物可利用性低，其潛在風險小。
沉積物生物毒性分析以效應百分比(PE)評估，結果顯示愛河口及第二港口沉積物毒性較低，而大部分測站沉積物呈現輕微以上的毒性反應，其中在前鎮河口及鹽水港溪口沉積物觀察到最高的生物毒性，表示其沉積物具有較高的危害。港區沉積物生物毒性程度空間分布依序為：河口> 航道> 港口。綜合三種化學評估方法與生物毒性結果顯示，雖然港區沉積物受到金屬污染，但由於港區富含硫化物，因此易被生物利用到的金屬含量少，大部分金屬移動性不高，現地沉積物中由金屬造成的毒性，可能性較小。

This study collected total of 60 surface sediment samples from the Kaohsiung Harbor in entrance (2 stations), the southern channel (6 stations), the northern channel (8 stations) and river estuary (4 stations) regions in January, April and July 2019. Analysis of physicochemical characteristics of sediments including: particle size distribution, total organic carbon (TOC), pH, oxidation-reduction potential (ORP), acid volatile sulfide (AVS) and heavy metals (including copper, lead, nickel, cadmium, zinc, chromium, manganese, and iron). Heavy metals were analyzed by three ways: total digestion, AVS simultaneous extraction metal (SEM) and sequential extraction procedure (SEP). Metal analysis results are further by the pollution load index (PLI), toxic risk index (TRI), equilibrium partitioning sediment benchmarks with AVS (ESBAVS OC), bioavailability index of metals (BI), and potential mobility index of metals (PMI) to evaluate the potential mobility and bioavailability of heavy metals in the harbor area. In addition, the sediment toxicity was confirmed by biological toxicity test (Microtox) and compared with the results of three metal chemical methods to comprehensively assess the potential toxicity of sediment heavy metals in the harbor area.
The total amount of metals in the sediments of the Kaohsiung Harbor that the concentration in copper is 8.57–858 mg/kg; lead is 10.2–90.8 mg/kg; nickel is 20.1–79.0 mg/kg; cadmium is 0.01–1.98 mg kg; zinc is 69.2–1367mg/kg; chromium is 17.1–249 mg/kg; manganese is 100–956 mg/kg. The total amount of metals in the sediments of the harbor area are spatially: river estuary> channel> entrance, indicating that the heavy metals in the sediments of the harbor area mainly come from the waste water injected with the upstream river. The results of sediment assessment indicators (PLI and TRI) based on the total amount of heavy metals show that the river estuary and channel sediments are polluted by a large amount of heavy metals from low to high level of metal toxicity risk. The entrance sediments are less polluted by heavy metals and the risk of toxicity is lower. According to the analysis results of AVS simultaneous extraction metal (SEM), the distribution of SEM is similar to the total metal , and clarify more than 75% of that. However, the sediments were further evaluated by the ESBAVS OC and it was found that the river estuary sediments are full in AVS (15.3–172 μmol/g) and TOC (1.12–7.69 %), that the divalent metal will combine with AVS to metal sulfides and that is not easy to dissolve, thus the river estuary sediments are seriously polluted by heavy metals, but its bioavailability is lower. The heavy metal pollution in the sediments of some channels and entrances is lower, but the AVS and TOC contents are also lower. The bioavailability of the heavy metal in the sediments is higher than that in the river estuary sediments. According to the SEP evaluation indicators (BI and PMI), the heavy metals in the sediments of Kaohsiung Harbor have found that some of the heavy metals in the sediments of the South Channel and the Salt River has potential mobility. Overall, the bioavailability of the heavy metals in the sediments of the harbor is lower, and the potential risk is slight.
Sediment biological toxicity analysis was evaluated by the percent effect (PE). The results exhibited that the sediments of Love River and Entrance II had no toxicity, and most of the station sediments exhibited slightly more levels of toxicity. The more biological toxicity was observed in the sediments of Jen-Gen River and Salt River, which indicated that the sediments had a higher hazard. The spatial distribution of the biological toxicity of sediments in the harbor area is in order: river estuary> channel> entrance. Comprehensive evaluation of the three extraction methods and the results of biological toxicity showed that although the sediments in the harbor area were severely polluted by heavy metals, but harbor area is rich in sulfides, the metals that can be easily used by organisms is small, and most of the metals are not highly mobile. The toxicity caused by metals in the on-site sediments is less likely.

摘要 i
Abstract iii
圖目錄 ix
表目錄 xi
第一章 前言 1
第二章 文獻回顧 4
2.1環境中金屬來源及宿命 4
2.2環境中金屬潛在危害之評估 5
2.2.1金屬總量 6
2.2.2酸揮發性硫化物/同步萃取金屬 11
2.2.3金屬鍵結型態 14
第三章 材料與方法 19
3.1 研究架構 19
3.2研究區域與測站規劃 21
3.2.1研究區域 21
3.3.1測站規劃 21
3.3 樣品採集及保存 24
3.4 試藥與設備 24
3.4.1 實驗藥品 24
3.4.2 試劑配製 26
3.4.3 實驗設備及儀器 28
3.5 樣品前處理及分析方法 29
3.6資料分析 39
3.6.1數據分析 39
3.6.2統計分析 40
第四章 品保品管 42
4.1 方法空白樣品 42
4.2 重複樣品分析 42
4.3 查核樣品分析 47
4.4 檢量線 52
4.5 準確度 53
4.6 偵測極限 55
第五章 結果與討論 60
5.1沉積物基本性質 60
5.2沉積物金屬總量分析 71
5.2.1金屬總量濃度時空分布 71
5.2.2沉積物金屬污染程度及潛在毒性風險評估 83
5.3 酸揮發性硫化物/同步萃取金屬分析 93
5.3.1酸揮發性硫化物/同步萃取金屬濃度時空分布 93
5.3.2評估沉積物金屬生物可利用性 103
5.4 金屬鍵結型態分析 107
5.4.1金屬各相態濃度分布 107
5.4.2評估沉積物金屬生物可利用性及潛在移動性 119
5.5沉積物生物毒性測試與化學評估結果之綜合探討 123
第六章 結論及建議 129
6.1 結論 129
6.2建議 130
參考文獻 131
附錄 160

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