臺灣博碩士論文加值系統

在台灣南部地區農民常在秋天稻草收割後，就地露天燃燒，此種燃燒行為會產生大量的黑炭，累積於土壤中。本實驗的目的在於估計台灣中南部地區農田的黑炭量，以及評估農田黑炭的含量對於除草劑之有效性與宿命是否會造成影響。
本論文測定土壤黑炭含量的方法，係先以酸去除土壤中的碳酸鹽，在充足的空氣中加熱375℃，再使用元素分析剩餘物質的碳元素；較佳的取出黑炭的方法，係使用化學分離再以比重分離，從土壤中取出密度為1.8至2.05 g/cm3的黑炭。研究中並使用吾人在農田裡自行燃燒稻草所產生的黑炭做比較；以達有龍水溶液作為吸附質，以批次的方法進行黑炭與土壤的等溫吸附實驗，並使用固相微萃取技術(SPME)配合氣相層析儀和電子捕捉偵測器作為量測水溶液濃度的工具。土壤的吸附量以dual-mode模式，並分別計算出黑炭及其他成分的吸附量對於土壤整體的吸附量所佔的比例，以評估黑炭的影響性。
從彰化線西土中，使用比重法分離出的黑炭比表面積為14 m2/g，碳元素含量為17%，自行燃燒稻草所產生的黑炭，其比表面積為78 m2/g，碳元素含量為14%，其比表面積差異的原因在於黑炭是否有經過長期在環境中馴化(aging)。
在彰化線西的土壤實驗裡，假設土壤吸附量為有機質和黑炭吸附所貢獻，使用dual-mode模式，扣除模擬比重分離的黑炭之吸附量，算出的達有龍對土壤有機質平衡係數(logKOC)為2.85 L/kg。由模擬結果顯示，黑炭吸附所佔的比例在吸附質濃度低時較大，且使用一地區所分離的黑炭，不適合模擬其他地區的土壤與黑炭吸附行為，黑炭之吸附量在達有龍濃度為1 mg/L時係佔土壤吸附量的64%。若達有龍被吸附後將會失去有效性，則黑炭含量對於除草劑的有效性及最適用量是有影響性的。

Farmers in Taiwan often open-burn their agriculture wastes on-site after harvesting in the autumn. This kind of burning practices produces a large amount of black carbon, which will be accumulated in the soils. The purpose of this study lies in estimating the black carbon amount of some areas in Taiwan, and its influence to the availability of pesticides in farmland soils.
This study developed the analytical method for the content of black carbon in soils by using weak acid to remove the carbonate in the soil, heating soil under 375 ℃ and sufficient air, and then measuring the carbon content of the left materials by element analysis. Black carbon was isolated by using chemical pretreatment and density fractionation by isolating the material with density between 1.8 and 2.05 g/cm3. Black carbon which we made by burning the straw was also investigated for comparison.
Diuron sorption by black carbon in aqueous solution was investigated by batch equilibration technology, extracting diuron by using solid-phase microextraction (SPME) method and measuring the concentration of the diuron aqueous solution by gas chromatograph equipped with electron capture detector.
The black carbon that isolated by density fractionation is from Hsienshi of Changhua county. The surface area is 14 m2/g , and the content of carbon is 17%. Surface area of the black carbon that produced by burned straw is 78 m2/g and the content of carbon is 14%.
A dual-mode model was used to simulate the adsorption of diuron on soil of Hsienshi of Changhua county, assuming that the adsorption of soil is contributed by sorption into organic matter and adsorption on black carbon. It is found that the amount of diuron adsorbed on the black carbon accounts for a large fraction of the amount sorbed on soil than organic matter does in low diuron concentration. Black carbon account for 64% of soil adsorbing capacity under the aqueous concentration of diuron at 1 mg/L.

中文摘要
英文摘要
第一章 緒論 1
1.1 前言 1
1.2 研究動機及目的 2
1.3 研究內容 3
第二章 研究背景與原理 4
2.1 黑炭(black carbon, BC)的概述 4
2.1.1 黑炭在環境中的分佈 5
2.1.2 黑炭的特性 5
2.1.3 黑炭在土壤中所扮演的角色 8
2.2 從土壤分離黑炭與定量方法 9
2.2.1直接觀察 10
2.2.2 化學氧化分離法 10
2.2.3 化學熱氧化(CTO)處理法 12
2.2.4 比重分離法 13
2.2.5 自行燃燒木頭和作物 14
2.3 除草劑簡介 15
2.3.1 有機化合物殺草劑之發展 15
2.3.2 達有龍(diuron) 15
2.4 固相微萃取技術(solid-phase microextraction, SPME) 18
2.4.1 固相萃取作為活性量測之發展與應用 18
2.4.2 PDMS的物化特性 19
2.4.3 SPME在環境上的應用 20
2.5 土壤之吸附現象 20
2.5.1 吸附(adsorption)與分配(partition) 20
2.5.2 土壤各成分的的吸附特性 21
2.5.3 黑炭形成時的差異性 24
2.5.4 黑炭的吸附特性 24
2.5.5 等溫吸附模式 25
2.5.6 常見之等溫吸附吸附經驗式 26
2.6 磁滯迴路(hysteresis loops) 29
第三章 研究方法 31
3.1 研究架構 31
3.2 實驗方法 32
3.2.1 吸附劑的取得 32
3.2.2 從土壤分離黑炭 33
3.2.3 土壤中黑炭含量的推估 33
3.2.4 元素分析 34
3.2.5 黑炭成分分析 34
3.2.6 比表面積測定及孔隙分佈分析 35
3.2.7 表面官能基的測定 35
3.2.8 黑炭與土壤對農藥的等溫吸脫附曲線和動力實驗 36
3.3 等溫吸附實驗 36
3.3.1 動力吸附實驗 37
3.3.2 量測水溶液中農藥濃度 37
第四章 結果與討論 40
4.1土壤中有機質與黑炭含量 40
4.2 土壤與稻草灰黑炭加熱後表面積與孔洞分析 42
4.3 黑炭的性質 43
4.4土壤及黑炭的孔隙分佈 45
4.4.1黑炭孔隙分佈 45
4.4.2土壤孔隙分佈 47
4.4.2各種黑炭的表面官能基 50
4.4.3黑炭與活性碳的表面構造 53
4.5 光纖和達有龍水溶液平衡時間及分析精密度 60
4.5.1上部空間的影響 61
4.6 稻草灰黑炭吸附達有龍之動力與平衡 61
4.7 平衡吸附係數與等溫脫附曲線 62
4.8 土壤與黑炭的等溫吸附曲線 63
4.8.1 自製黑炭與從土壤分離黑炭之等溫吸附曲線 63
4.8.2 土壤之等溫吸附曲線 65
4.8.3 土壤有機質之吸附量 66
4.8.4 稻田中黑炭對吸附除草劑之貢獻量 70
第五章 結論與建議 71
參考文獻 73





圖目錄
圖2.1達有龍的分子結構 17
圖2.2土壤中對於非極性有機化合物被吸附之五種方式示意圖 22
圖2.3等溫吸附曲線類型 26
圖2.4 磁滯曲線類型 30
圖3.1實驗架構圖 31
圖4.1稻田上收集灰的孔隙分佈曲線 46
圖4.2稻草灰黑炭與經過加熱處理後的孔隙分佈圖 46
圖4.3 活性炭的孔隙分佈圖 47
圖4.4 彰化土分離出的黑炭孔隙分佈圖 47
圖4.5 (a)彰化線西土壤孔隙分佈曲線 (b)雲林崙背土壤孔隙分佈曲線 48
圖4.6 (a)嘉義義竹土壤孔隙分佈曲線 (b)嘉義朴子壤孔隙分佈曲線 49
圖4.7 (a)稻草灰黑炭FTIR光譜 (b)活性碳FTIR光譜 51
圖4.8 (a)從土壤中分離的黑炭FTIR光譜(沒有使用氫氟酸) (b) 從土壤中分離的黑炭FTIR光譜(有使用氫氟酸) 52
圖4.9 自行燃燒稻草所生成的稻草灰黑炭電子顯微鏡拍攝圖(a)×1800與 (b)×4000 54
圖4.10活性碳電子顯微鏡拍攝圖(a)×1000與(b)×3000 55
圖4.11 從雲林崙背土分離出的黑炭(YL-A-B-D) (a)×3000與(b)×800 56
圖4.12 從彰化線西土分離出的黑炭(CS-A-B-D) (a)×1000與(b)×1500 57
圖4.13 從彰化線西土分離出的黑炭(CS-A-F-E-B-D) (a)×2000與(b)×3000 58
圖4.14 從雲林崙背土分離出的黑炭(YL-A-F-E-B-D) (a)×2000與(b)×10000 59
圖4.15光纖吸附達有龍之動力試驗結果 60
圖4.16 稻草灰黑炭吸附達有龍之動力曲線圖。 62
圖4.17 稻草灰黑炭與達有龍水溶液濃度之動力吸脫附曲線圖 63
圖4.18 稻草灰黑炭與達有龍之脫附動力曲線圖 63
圖4.19以CS-A-B-C所分離之黑炭與達有龍水溶液的等溫吸附曲線 64
圖4.20 稻草灰黑炭與達有龍水溶液的等溫吸附曲線。 64
圖4.21 以dual-mode model模擬圖彰化線西土(a) 以自行燃燒的稻草灰黑炭模擬(b)以CS-A-B-D分離出之黑炭模擬 68
圖4.22 以dual-mode model模擬(a)嘉義朴子土 (b)嘉義義竹土 (c)雲林土壤吸附量 69



表目錄
表2.1 不同黑炭的比較 4
表2.2黑炭物質的比重 6
表2.3黑炭的元素組成 7
表2.4 各種定量和分離黑炭方法的優缺點 14
表2.5 稻草及小麥飛灰之元素分析 15
表2.6 達有龍的物化性質 17
表2.7土壤中五種成分對於非極性有機化合物之吸脫附機制及動力的定性比較 23
表3.1採樣地座標 32
表3.2光纖性質 38
表4.1 處理方法與土壤代號表 40
表4.2土壤中黑炭與有機質含量 41
表4.3 彰化土分離出的黑炭比例及比表面積 41
表4.4土壤及稻草灰經加熱處理後的比表面積與孔隙 42
表4.5各種黑炭的元素分析 43
表4.6各種黑炭之比表面積及孔隙寬度 45
表4.7光纖重複分析之相對差異 60
表4.8不同上部空間測得之濃度與相對差異表 61
表4.10 黑炭等溫吸附模擬參數表 65
表4.11土壤與達有龍之等溫吸附參數 66
表4.12以扣除黑炭吸附量後之實驗值推算各土壤中的KOC值 67
表4.13 各濃度黑炭吸附量與總吸附量的比例 70

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