臺灣博碩士論文加值系統

河川底泥具有高累積污染物的能力，因而被認為是污染物的匯聚池。重金屬具不易生物降解的特性，因而廣受關注，且底泥重金屬之生物有效性可能受底泥特性、底泥—水交介面傳輸行為及水生生物生理性質影響。為了解底泥中重金屬與水生生物間的化學及生物作用，此研究使用流水式全底泥暴露系統，將青鱂魚幼魚及胚胎同時暴露於銅及鉛污染底泥達七天，以評估污染底泥對於不同時期魚類之生物有效性及毒性，以及銅及鉛間傳輸與影響。四種環境底泥之基本性質迥異，其中中正橋底泥(ZZ)及外雙溪底泥(WS)屬於粗質地之砂土，淡水河底泥(TS)屬於中質地之壤質砂土，而萬板大橋底泥(WB)屬於細質地的壤土。WB之陽離子交換容量(CEC)最高，而WB及TS之有機碳含量(OC)較ZZ及WS高。此外，pH由高至低分別為TS > WS > ZZ > WB。研究結果顯示，幼魚暴露於四種銅及鉛污染底泥之毒性均高於胚胎。在銅及鉛污染之中，ZZ暴露下幼魚及胚胎均有最高的死亡率，而TS之死亡率最低，顯示粗質地、低pH等底泥性質，會增加底泥之金屬釋放能力。此外，幼魚之體長及體重在所有銅及鉛污染底泥暴露下皆顯著被抑制；相反的，胚胎之孵化率在所有底泥處理組中，未呈現劑量反應關係，證實在污染底泥系統中，青鱂魚幼魚對於毒性之反應較胚胎更為敏感。銅污染或鉛污染底泥處理組[500 mg-Cu/kg (500/0)及500 mg-Pb/kg (0/500)]之幼魚存活率皆較銅及鉛污染底泥處理組[250-Cu/250-Pb mg/kg (250/250)]低。然而，當銅污染底泥及銅及鉛處理組中銅濃度接近時，幼魚之存活率卻有相近的趨勢，因此，幼魚之致死毒性主要貢獻於銅，因底泥較易釋放銅至水相中，而鉛在底泥中的生物有效性較低。本研究以log-logistic模型或線性迴歸模型進行化學指標如底泥金屬總量、水相（表層水、孔隙水）溶解態金屬濃度以及Chelex-100樹脂抽出量與生物毒性及生物有效性之相關分析。其中，Chelex-100樹脂抽出量對於銅及鉛污染底泥之生物體內金屬含量與毒性均具有最好的預測能力，而孔隙水最差。因此，Chelex-100樹脂抽出法能夠作為預測底泥重金屬污染之生物有效性及毒性的化學評估方法。

In the river system, sediment is considered as a long-term source of contaminants for aquatic organisms due to its high accumulating capacity. Among all contaminants, heavy metals are of high concern because of their non-biodegradable nature. The bioavailability of these metals may be affected by sediment properties, transportation behavior between sediment-water system and physiology of aquatic organisms. To understand the chemical and biological interaction of sediment-bound contaminants to the aquatic life, this study used the whole-sediment exposure method with intermittent water renewal system to evaluate the bioavailability and toxicity of two heavy metals [i.e. lead (Pb) and copper (Cu)]. Medaka (Oryzias latipes) embryos and larvae, which were used as model organisms, were exposed to a variety of Pb- and Cu-spiked sediments with different physicochemical properties for 7 days to evaluate the toxicity and bioavailability. Moreover, this study discussed the transportation and effect in the sediment between these two metals. The physiochemical properties of four sediments were totally different. ZZ sediment and WS sediment were sand, TS sediment was loamy sand and WB was loam. In these sediments, WB had the highest CEC, as well as ZZ and WS has lower OC. pH value from high to low were TS > WS > ZZ > WB. Survival rates of both treated embryos and larvae from TS were the highest, and those from ZZ were the lowest. As such, we believed that metals in lower pH, CEC, OC and more sandy sediment were more releasable, and larvae were more sensitive to metal toxicity than embryos. Moreover, the larval morphology i.e. body length and body weight in dual metal spiked sediments groups were significantly inhibited in very low concentrations. The trend of larval mortality spiked with single Cu into ZZ sediment was similar to that with dual metal at in same Cu concentration. Based on the results, the lethal toxicity was mainly affected by Cu, as the bioavailability of Pb was low. In this study, we also used several analytical approaches to assess the bioavailability of these two metals and the correlation (log-logistic model and linear regression) with observed toxic effects. The resuls showed that Chelex-100 resin extraction method can be an effective method for predicting and evaluating bioavailability of sedimental Cu and Pb to medaka no matter in single or dual metal polluted sediment.

致謝 I
中文摘要 II
ABSTRACT IV
縮寫對照表 VI
目錄 VII
圖目錄 XI
表目錄 XIII
第一章 前言與研究動機 1
第二章 文獻回顧 2
2.1 污染物在環境之流布 2
2.1.1 銅污染來源及生物毒性 3
2.1.2 鉛污染來源及生物毒性 4
2.2 重金屬在水生系統中的型態 5
2.2.1 銅在底泥及水相中的型態 5
2.2.2 鉛在底泥及水相中的型態 7
2.3 底泥中重金屬風險評估及生物有效性評估之方法 9
2.3.1 序列萃取法 11
2.3.2 水相溶解態金屬含量 12
2.3.3 Chelex-100樹脂吸附法 13
2.3.4 生物金屬累積量 14
2.3.5 生物毒性檢測法 15
2.4 模式生物—青鱂魚 16
2.5 研究之創新及目的 17
2.5.1 知識缺口 17
2.5.2 研究目的 18
第三章 材料與方法 19
3.1 研究架構說明 19
3.2 實驗器材 21
3.2.1 藥品與試劑 21
3.2.2 儀器設備 22
3.3 底泥採樣及基本性質分析 23
3.3.1 採樣地點及前處理方式 23
3.3.2 底泥基本性質分析 26
3.3.2.1 酸鹼值 26
3.3.2.2 氧化還原電位 26
3.3.2.3 飽和含水量 26
3.3.2.4 陽離子交換容量 26
3.3.2.5 質地 27
3.3.2.6 飽和水電導度 27
3.3.2.7 有機碳含量 28
3.3.2.8 常見重金屬含量 28
3.4 7日流水式全底泥暴露試驗 29
3.4.1 流水式底泥暴露系統 29
3.4.2 銅及鉛污染底泥配置 31
3.4.3 青鱂魚馴養及試驗胚胎收集 33
3.4.3.1 成魚馴養條件 33
3.4.3.2 試驗胚胎挑選 34
3.4.3.3 試驗幼魚馴養 34
3.4.4 污染底泥生物暴露試驗 36
3.5 流水式全底泥暴露系統之金屬含量分析 39
3.5.1 底泥重金屬總量分析 39
3.5.2 溶解態金屬含量分析 40
3.5.2.1 表層水金屬濃度分析： 40
3.5.2.2 孔隙水金屬濃度分析： 40
3.6 以Chelex-100樹脂吸附法抽出底泥之生物有效金屬 41
3.6.1 Chelex-100樹脂袋製備 41
3.6.2 Chelex-100樹脂袋暴露方式 41
3.7 生物毒性指標測量 43
3.7.1 胚胎生物毒性指標 43
3.7.1.1 胚胎存活率 43
3.7.1.2 胚胎孵化率 43
3.7.1.3 胚胎心搏數 43
3.7.1.4 胚胎孵化之魚苗體內金屬含量 44
3.7.2 幼魚生物毒性指標 45
3.7.2.1 幼魚存活率 45
3.7.2.2 幼魚體長抑制率 45
3.7.2.3 幼魚體重抑制率 45
3.7.2.4 幼魚體內金屬含量 45
3.8 統計分析 46
第四章 結果與討論 47
4.1 環境底泥基本性質分析結果 47
4.2 全底泥暴露系統之最佳化流水式 51
4.2.1 污染底泥平衡時間選擇 51
4.2.2 試驗暴露時間起點選擇 51
4.3 中正橋(ZZ)銅、鉛污染之全底泥暴露試驗結果 53
4.3.1 中正橋銅或鉛污染底泥之化學分析結果 53
4.3.1.1 生物暴露前表層底泥銅、鉛含量 53
4.3.1.2 生物暴露試驗期間表層水中銅、鉛釋出量 53
4.3.1.3 第7日底泥孔隙水中金屬濃度 56
4.3.1.4 Chelex-100樹脂抽出銅、鉛含量 56
4.3.2 中正橋銅或鉛污染底泥之生物毒性結果 59
4.3.2.1 暴露於銅或鉛汙染底泥之青鱂魚胚胎致死毒性結果 59
4.3.2.2 暴露於銅或鉛汙染底泥青之鱂魚胚胎孵化率結果 59
4.3.2.3 經銅或鉛汙染底泥暴露後胚胎孵化之魚苗中銅及鉛含量 61
4.3.2.4 銅或鉛汙染之中正橋底泥(ZZ)對青鱂魚幼魚之致死毒性比較 63
4.3.2.5 銅或鉛汙染之中正橋底泥(ZZ)對青鱂魚幼魚之發育毒性比較 63
4.4 流水式全底泥暴露試驗銅及鉛污染底泥化學分析結果 66
4.4.1 生物暴露試驗前之表層底泥銅、鉛總體濃度分析結果 66
4.4.2 生物暴露試驗期間之表層水中銅、鉛釋出量變化 66
4.4.3 底泥生物暴露第7日底泥孔隙水中銅、鉛金屬濃度 71
4.4.4 Chelex-100樹脂於流水式全底泥暴露系統48小時期間抽出量 75
4.5 7日流水式全底泥之胚胎暴露試驗結果 78
4.5.1 四種銅及鉛污染底泥對青鱂魚胚胎之致死毒性 78
4.5.2 四種銅及鉛污染底泥對青鱂魚胚胎之發育毒性 80
4.5.2.1 第7日胚胎心搏數 80
4.5.2.2 胚胎孵化率 80
4.5.2.3 胚胎孵化之魚苗體內銅及鉛含量 83
4.6 7日流水式全底泥之幼魚暴露試驗結果 85
4.6.1 四種銅及鉛污染底泥對青鱂魚幼魚之致死毒性 85
4.6.2 四種銅及鉛污染底泥對青鱂魚幼魚生長之干擾 87
4.6.2.1 幼魚生長抑制率 87
4.6.2.2 幼魚體內銅及鉛含量 90
4.7 污染底泥中銅及鉛釋放能力及生物有效性探討 93
4.7.1 銅、鉛及銅鉛混合污染底泥之化學效應評估 93
4.7.1.1 表層水中溶解態銅、鉛濃度比較 93
4.7.1.2 孔隙水中溶解態銅及鉛濃度比較 94
4.7.1.3 Chelex-100從污染底泥抽出之銅及鉛含量比較 94
4.7.2 銅、鉛及銅鉛混合污染底泥之生物效應評估 96
4.8 多種化學方法與生物反應之相關性分析結果 99
4.8.1 不同化學方法對生物毒性之預測能力 99
4.8.1.1 樹脂銅及鉛抽出量與流水式全底泥暴露試驗幼魚存活率之關係 99
4.8.1.2 水相銅及鉛濃度與流水式全底泥暴露試驗幼魚存活率之關係 100
4.8.1.3 底泥銅及鉛總量與流水式全底泥暴露試驗後幼魚存活率之關係 101
4.8.2 不同化學方法對生物體內金屬含量之預測 104
4.8.2.1 樹脂銅及鉛抽出量與全底泥暴露試驗後幼魚體內銅及鉛含量之關係 104
4.8.2.2 水相銅及鉛濃度全底泥暴露試驗後幼魚體內銅及鉛含量之關係 105
4.8.2.3 底泥金屬總量與全底泥暴露試驗幼魚生物體內金屬含量之關係 105
第五章 結論與建議 110
第六章 參考文獻 112 

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