本研究係以生物淋溶法來探討底泥中重金屬溶出之可能性。藉由二仁溪底泥中所馴養出之
原生硫氧化菌作為生物淋溶所需之微生物，在各種控制條件下(包括基質與接種體的添加、
接種百分比、基質濃度、總固體物濃度、溫度)，將底泥中硫化物或額外添加還原態硫化物
氧化，以形成硫酸進而溶出底泥中重金屬。此外，本研究也以逐步萃取法(sequential
extraction procedure, SEP)分析並探討底泥中重金屬各鍵結型態組成(包括可交換態，與
碳酸鹽鍵結態，與錳氧化物鍵結態，與鐵氧化物鍵結態以及與有機物鍵結態)，在生物淋溶
前後之變化。
本研究結果顯示，在生物淋溶過程中，底泥溶液pH值逐漸下降，氧化還原電位則逐漸上升
，底泥中硫化物及添加之硫代硫酸鈉逐漸氧化成硫酸鹽，而總可萃取重金屬之溶出效率也
隨之增加。
在基質與接種體的添加的試驗中，發現接種體對底泥溶液pH值降低之影響比硫添加的影響
為高。在不同接種百分比的淋溶試驗中則顯示，高接種百分比能使pH值的下降較快。經生
物淋溶後，總可萃取重金屬的平均溶出效率之次序為鋅、銅、鎳＞鉻＞鈷＞鉛。除了鈷與
鎳以外，鉻、鋅、銅和鉛鍵結型態之分佈在淋溶前後皆較有一致性的分佈變化。
在不同基質濃度的生物淋溶試驗中，發現當基質濃度小於4.80 g S/L時，隨著基質濃度含
量增加時，其底泥溶液最終pH值也隨之下降。當基質濃度大於4.80 g S/L時，硫氧化菌之
生物氧化作用可能受到抑制，因而使得底泥溶液pH值無法下降。總可萃取重金屬之溶出效
率以基質濃度含量為4.80 g S/L時最佳，其中以鋅的溶出效率為最高，鉛之溶出率則最低
。
總固體物之含量(TS)可表示為底泥的緩衝能力。結果發現，此值明顯影響底泥溶液中pH值
之下降速率。當總固體物含量愈低時，底泥溶液pH值之下降速率愈大。經生物淋溶後，不
同重金屬在不同的總固體物含量下，有不同的鍵結行為。
在不同控制溫度的淋溶試驗中顯示，硫氧化菌氧化活性在37.0 ℃時最為明顯。除了鉛以外
，其他重金屬從各鍵結位置之溶出率在37.0 ℃時最高，25.0 ℃時溶出率稍差，而在55.0
℃時之溶出效率則明顯最差。溫度變化對生物淋溶前後各種重金屬鍵結型態之變化有顯著
性的影響。在55.0 ℃時，六種重金屬各鍵結型態間之重新分佈現象最為明顯。

The aim of this study is to explore the mobility of heavy metals from
contaminated river sediments by using bioleaching process. Indigenous sulfur-
oxidizing bacteria (SOB) enriched from the sediments of Ell-Ren river were
used to oxidize the reduced sulfur originally existed in sediments or added to
sulfuric acid under controlled operational conditions (including percentage of
inoculum, percentage of substrate added, total solid content and temperature),
which resulted in the mobilization of heavy metals from contaminated
sediments. In addition, the changes in metal binding characteristics that
occur during bioleaching will be explored by using sequential extraction
procedure.
Due to the production of sulfuric acid from the oxidation of reduced sulfur,
the accompanying increase of sulfates, decrease of pH and increase of mobility
of total extractable heavy metals were found.
Results show that the effect of inoculum adding on pH decrease was more than
that of sulfur adding. Higher inoculum percentage could speed up the decrease
of pH more during bioleaching. The order of mobilization of total extractable
heavy metals (TEHMS) could be shown as following: Zn, Cu, Ni＞Cr ＞Co＞Pb.
Except for Co and Ni, the binding fractions of other heavy metals had a
consistent variation after bioleaching.
It was found that the sediment pH decreased with the increase of substrate
concentration while it was lower than 4.80 gS/L. When the concentration of
substrate was higher than 4.80 gS/L, the sediment pH could not drop down,
which might be due to the inhibition of biochemical reaction. The optimum
dosage of substrate for mobilizing TEHM was found at 4.80 gS/L.
The total sediment solids (TS) represent the buffer capacity of sediment.
Consequently, a lower TS leads to a easier likelihood of overcoming the
sediment buffer, and hence a lower sediment pH. Different heavy metals showed
different binding behavior at the various TS concentrations.
Of three temperatures tested (25.0℃, 37.0℃ and 55.0℃), pH decrease was
greatest at 37.0℃, indicating that, after acclimation, bacterial oxidizing
activity is greatest at this temperature. Except for Pb, the optimal
temperature for solubilization of total extractable heavy metal was 37.0℃.
The temperature of bioleaching had a significant impact on changes in
partitioning of heavy metals. Transfer of heavy metals between binding
fractions was most apparent at 55.0℃ before and after bioleaching.

中文摘要.......................................................I
英文摘要.....................................................III
誌謝...........................................................V
目錄..........................................................VI
表目錄........................................................XI
圖目錄......................................................XIII
第一章 緒論....................................................1
1.1 研究動機...................................................1
1.2 研究目的...................................................2
第二章 文獻回顧................................................5
2.1 底泥的意義.................................................5
2.1.1 底泥的定義...............................................5
2.1.2 底泥的形成...............................................5
2.1.3 底泥的組成...............................................6
2.2 底泥研究的重要性...........................................6
2.2.1 底泥污染的意義...........................................6
2.2.2 受重金屬污染之底泥對水體環境的影響.......................7
2.2.3 底泥品質評估.............................................8
2.2.3.1 底泥品質標準之建立.....................................8
2.2.3.2 底泥品質評估方法.......................................8
2.3 底泥的管理策略.............................................9
2.4 底泥中重金屬的意義........................................10
2.4.1 底泥中重金屬鍵結機制....................................10
2.4.2 金屬在底泥中鍵結型態....................................12
2.4.3 底泥中鍵結型態之來源及其移動性..........................15
2.4.4 金屬鍵結型態在環境上的意義..............................16
2.5 底泥中污染物的去除方法....................................18
2.5.1 底泥中污染物的種類......................................18
2.5.2 受污染之底泥的處理方法..................................18
2.5.2.1 底泥現地處理法........................................18
2.5.2.2 底泥非現地處理法......................................20
2.5.3 底泥中重金屬的去除方法..................................22
2.6 以生物淋溶法去除底泥中重金屬..............................25
2.6.1 生物淋溶之原理..........................................25
2.6.1.1 直接機制(direct mechanism)............................25
2.6.1.2 間接機制(indirect mechanism)..........................26
2.6.2 硫化桿菌屬(Thiobacillus)之生物特性......................27
2.6.3 生物淋溶的影響因素......................................29
2.6.4 生物淋溶之應用..........................................29
2.6.4.1 在採礦冶金之應用......................................32
2.6.4.2 在污泥重金屬的去除處理上之應用........................32
2.6.4.3 在底泥重金屬的去除處理上之應用........................33
第三章 實驗設備、材料與方法...................................37
3.1 研究流程..................................................37
3.2 實驗設備及儀器............................................39
3.3 實驗材料及藥品............................................40
3.4 底泥樣品的採集............................................41
3.5 底泥之物化特性分析........................................41
3.5.1 底泥物化特性分析方法....................................42
3.6 原生硫氧化菌之馴養........................................45
3.6.1 馴養方法及步驟..........................................45
3.7 生物淋溶試驗..............................................46
3.7.1 生物淋溶試驗方法及步驟..................................46
3.7.2 生物淋溶試驗實驗分析項目及方法..........................46
3.7.3 生物淋溶試驗操作條件之探討..............................47
3.7.3.1 基質和接種體的添加對生物淋溶試驗之影響................47
3.7.3.2 不同接種百分比(v/v)對生物淋溶試驗之影響...............48
3.7.3.3 不同基質濃度對生物淋溶試驗之影響......................48
3.7.3.4 不同固體物濃度對生物淋溶試驗之影響....................48
3.7.3.5 不同溫度對生物淋溶試驗之影響..........................49
3.8 底泥中重金屬鍵結型態之分析................................49
3.8.1 逐步萃取法操作條件與流程................................50
第四章 結果與討論.............................................54
4.1 底泥之物化特性分析........................................54
4.1.1 泥樣A之物化特性分析.....................................54
4.1.2 泥樣B之物化特性分析.....................................58
4.2 原生硫氧化菌馴養..........................................62
4.2.1 馴化過程中底泥pH值之變化................................62
4.2.2 底泥的添加對生物淋溶試驗中pH值變化之影響................64
4.2.3 底泥的添加對生物淋溶試驗中氧化還原電位變化之影響........65
4.2.4 底泥的添加對生物淋溶試驗中硫酸鹽變化之影響..............66
4.3 基質和接種體的添加對硫氧化菌淋溶效果之影響................68
4.3.1 基質與接種體的添加對底泥pH值與硫酸鹽含量之影響..........68
4.3.2 基質與接種體的添加對總可萃取重金屬(TEHM)溶出效率之影響..70
4.3.3 基質與接種體的添加對生物淋溶前後重金屬鍵結型態變化之影響72
4.4 接種百分比對硫氧化菌淋溶效果之影響........................80
4.4.1 接種百分比對底泥pH值變化之影響..........................80
4.4.2 接種百分比對底泥氧化還原電位變化之影響..................82
4.4.3 接種百分比對底泥硫酸鹽含量變化之影響....................83
4.4.4 接種百分比對總可萃取重金屬(TEHM)溶出效率之影響..........84
4.4.5 接種百分比對生物淋溶前後重金屬鍵結型態變化之影響........86
4.5 基質濃度對硫氧化菌淋溶效果之影響..........................94
4.5.1 不同基質濃度對底泥pH值變化之影響........................94
4.5.2 不同基質濃度對底泥氧化還原電位變化之影響................96
4.5.3 不同基質濃度對底泥硫酸鹽含量變化之影響..................97
4.5.4 比較本研究與文獻其他研究中基質濃度對生物淋溶法之影響....99
4.5.5 不同基質濃度對總可萃取重金屬(TEHM)溶出效率之影響.......100
4.5.6 不同基質濃度對生物淋溶前後重金屬鍵結型態變化之影響.....101
4.6 總固體物含量對硫氧化菌淋溶效果之影響.....................111
4.6.1 總固體物含量對底泥pH值變化之影響.......................111
4.6.2 總固體物含量對底泥氧化還原電位變化之影響...............112
4.6.3 總固體物含量對底泥硫酸鹽含量變化之影響.................113
4.6.4 比較本研究與文獻其他研究中固體物含量對生物淋溶法之影響.116
4.6.5 總固體物含量對總可萃取重金屬(TEHM)溶出效率之影響.......116
4.6.6 總固體物含量對生物淋溶前後重金屬鍵結型態變化之影響.....118
4.7 溫度對硫氧化菌淋溶效果之影響.............................123
4.7.1 溫度對底泥pH值變化之影響...............................123
4.7.2 溫度對底泥氧化還原電位變化之影響.......................125
4.7.3 溫度對底泥硫酸鹽含量變化之影響.........................126
4.7.4 比較本研究與文獻其他研究中溫度對生物淋溶法之影響.......127
4.7.5 溫度對總可萃取重金屬(TEHM)溶出效率之影響...............128
4.7.6 溫度對生物淋溶前後重金屬鍵結型態變化之影響.............130
第五章 結論..................................................135
第六章 建議與未來方向........................................138
第七章 參考文獻..............................................139

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