臺灣博碩士論文加值系統

中文摘要
本研究主要利用不同廢棄生質(產氫麥粕與稻殼)做為起始原料，配合碳化及活化程序生成具有微孔孔隙之活性碳吸附劑，並經由硫含浸程序，以期應用此類吸附劑於微量汞吸附。在碳化溫度400°C，60 min，100% N2，與活化溫度800°C，10−90 min，50% H2O/50% N2下，可生成400−700 m2/g比表面積，350−500 m2/g微孔表面積，且具有0.8 nm尖峰孔徑之活性碳吸附劑。吸附劑之微孔表面積約佔比表面積之70%，且孔徑集中分佈於0.5−1 nm間，顯示廢棄生質合成微孔吸附劑之可行性極高。硫含浸處理(300−650°C)減低吸附劑之比表面積，主要由於硫分子進入吸附劑孔洞所致，且吸附劑經硫含浸處理後，微孔表面積與體積隨著含浸溫度下降而下降，但中孔與大孔結構於含浸溫度>400°C時受到較少影響，顯示硫分子於中高溫時傾向進入吸附劑微孔結構。XPS微區C1s、S2p峰值之表面官能基解析結果顯示，隨著硫含浸溫度下降，含氧官能基(hydroxyl, carbonyl, carboxyl) 隨著硫含浸溫度的下降而有減少的趨勢；而有機硫官能基(thiophene, sulfoxide, sulfone) 隨著硫含浸溫度的下降則有增加的趨勢。
經由表面改質硫含浸處理後的活性碳吸附劑對Hg0蒸氣的吸附能力均較原樣提升，且產氫廢麥粕活性碳對Hg0蒸氣的吸附效果皆略優於稻殼與商用活性碳(以中溫400°C的吸附量最為明顯)。擬二階吸附動力模式可獲得最佳之模擬結果(R2>0.989)，暗示Hg0吸附傾向於雙分子反應。此外幾乎本研究中所有具有高飽和吸附量之硫含浸活性碳，其反應動力均不佳，顯示硫含浸活性碳之吸附平衡與吸附動力並無顯著相關。

Abstract
This study evaluates the feasibility of developing low-cost sulfur-containing microporous adsorbents from agricultural byproducts for removal of low-concentration gaseous mercury. Various agricultural byproducts (i.e., hydrogen-generated wheat husk and rice husk) were used to develop activated carbons with carbonization (400°C, 60 min, 100% N2) and activation (800°C, 10−90 min, 50% H2O /50% N2) processes. The resulting samples possessed specific surface area of 400−700 m2/g, micropore area of 350−500 m2/g, and had a narrow pore-size distribution (pore sizes between 0.5 and 1 nm) with a peak at 0.8 nm. These results demonstrate the feasibility of producing microporous carbonaceous adsorbents using agricultural byproducts with suitable carbonization and activation. Sulfur impregnation (300−650°C) decreased the specific surface area of adsorbents, indicating that sulfur molecules accessed into the porous structure of adsorbents. Also, the microporous surface area and volume decreased as the sulfur impregnation temperature decreased. The mesoporous and macroporous structure of adsorbents, however, was less affected at sulfur impregnation at temperatures >400°C. These results suggest that sulfur molecules tend to enter the microporous structure at middle and high temperature ranges. Results from the examination of X-ray photoelectron spectroscopy showed that the contents of oxygen functional groups (i.e., hydroxyl, carbonyl, and carboxyl) decreased as sulfur impregnation temperature decreased. In contrast, the contents of sulfur functional groups (i.e., thiophene, sulfoxide, sulfone) increased as sulfur impregnated temperature decreased.
Sulfur impregnation resulted in an increase in the Hg0 adsorption capacities of carbonaceous adsorbents. The adsorbents derived from hydrogen-generated wheat husk typically had larger adsorption capacities than those of rice husk derived carbons and the commercial activated carbon. Results also showed that a pseudo-second-order model can successfully simulate the adsorption behaviors of all tested adsorbents (R2>0.989), indicating that Hg0 adsorption by tested samples was in a bimolecular reaction form. In addition, kinetic study also showed that the tested samples with large adsorption capacities typically had poor adsorption kinetics, indicating that the Hg0 adsorption equilibrium and kinetics of sulfur-impregnated activated carbon were not able to be well correlated.

目錄
中文摘要.............................................................................................................i
Abstract.............................................................................................................ii
誌謝...................................................................................................................iii
目錄...................................................................................................................iv
符號說明...........................................................................................................xi
一、前言............................................................................................................1
1.1 研究緣起.................................................................................................................1
1.2 研究目的.................................................................................................................3
二、文獻回顧....................................................................................................4
2.1 汞污染物的來源.....................................................................................................4
2.1.1 燃料燃燒....................................................................................................8
2.1.2 都市及醫療廢棄物焚化爐......................................................................10
2.1.3 化學工廠..................................................................................................14
2.1.4 電器或電子設備......................................................................................14
2.1.5 塗料、紙漿..............................................................................................14
2.1.6 石灰與水泥..............................................................................................14
2.2 汞之基本性質與傳輸途徑...................................................................................15
2.3 汞對人體健康的危害...........................................................................................17
2.3.1 金屬汞......................................................................................................18
2.3.2 無機汞......................................................................................................19
2.3.3 有機汞......................................................................................................19
2.4 燃煤過程中產生的汞物種與對應之防治技術...................................................19
2.4.1 吸附劑噴入..............................................................................................18
2.4.2 袋濾式活性碳床......................................................................................19
2.4.3 濕式煙道脫硫設備..................................................................................19
2.5 活性碳的用途.......................................................................................................20
2.6 活性碳概述...........................................................................................................21
2.6.1 比表面積(specific surface area)...............................................................21
2.6.2 孔隙結構(pore structure).........................................................................22
2.6.3 活性碳表面官能基..................................................................................22
2.7 活性碳的種類.......................................................................................................26
2.7.1 粉末狀活性碳(Powder Activated Carbon, PAC).....................................26
2.7.2 粒狀活性碳(Granular Activated Carbon, GAC)......................................26
iv
2.7.3 球形或圓柱形活性碳(Spherical or Cylindrical Activated Carbon)........26
2.7.4 活性碳纖維(Activated Carbon Fiber, ACF)............................................27
2.7.5 含浸活性碳(Impregnated Activated Carbon, IAC).................................27
2.8 活性碳吸附原理...................................................................................................28
2.8.1 吸附之熱力特性......................................................................................29
2.8.2 吸附機制..................................................................................................30
2.8.3 等溫吸附曲線..........................................................................................33
2.8.4 吸附遲滯(Hysteresis loop).......................................................................34
2.8.5 吸附過程..................................................................................................37
2.8.6 吸附模式..................................................................................................38
2.9 微孔吸附劑含浸處理後之吸附效果評估...........................................................40
三、研究材料與實驗方法..............................................................................47
3.1 研究材料與來源...................................................................................................47
3.2 實驗設備...............................................................................................................47
3.2.1 活性碳製程設備......................................................................................47
3.2.2 分析用設備..............................................................................................50
3.2.3 吸附實驗裝置..........................................................................................51
3.3實驗方法................................................................................................................55
3.3.1 活性碳合成實驗......................................................................................55
3.3.2 活性碳吸附實驗......................................................................................58
3.3.3 活性碳吸附實驗物化特性分析..............................................................58
3.3.4 比表面積、孔體積與孔徑分佈測定......................................................58
3.3.5 表面觀察..................................................................................................60
3.3.6 元素分析..................................................................................................60
3.3.7 表面官能基分析......................................................................................61
第四章、結果與討論......................................................................................62
4.1 活性碳物理特性分析結果...................................................................................62
4.1.1 等溫吸附曲線..........................................................................................64
4.1.2 BET比表面積與微孔表面積...................................................................68
4.1.3 孔體積......................................................................................................69
4.1.4 孔徑分佈..................................................................................................70
4.1.5 SEM表面觀察..........................................................................................74
4.2 活性碳化學特性分析結果...................................................................................78
4.2.1 元素分析結果..........................................................................................78
4.2.2 XPS化學表面官能基分析.......................................................................80
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4.3 活性碳吸附實驗結果...........................................................................................92
4.4 活性碳吸附動力分析...........................................................................................97
4.4.1 Pseudo-First Order Equation....................................................................99
4.4.2 Pseudo-Second Order Equation..............................................................100
4.4.3 Elovich Equation....................................................................................101
4.4.4 活性碳孔隙擴散模式............................................................................111
第五章、結論與建議....................................................................................121
5.1 結論.....................................................................................................................121
5.2 建議.....................................................................................................................122
參考文獻........................................................................................................124
附錄A.............................................................................................................133
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表目錄
表2.1 不同研究所估算之全球天然與人為汞排放量(UNEP, 2002).............................5
表2.2 不同排放源之全球汞排放量(UNEP, 2002).........................................................6
表2.3 全球各洲以人為排放源分類之汞排放量(UNEP, 2002).....................................7
表2.4 美國之人為汞排放量(Hasselriis, 1996)................................................................8
表2.5 燃煤組成成份一覽表(Galbreath and Zygarlicke, 2000; Gibb et al., 2000)..........9
表2.6 都市垃圾廢棄物組成對於汞重金屬之貢獻量(Rigo, 1993)..............................11
表2.7 美國大型垃圾焚化廠中汞的來源(Rigo, 1993)..................................................13
表2.8 汞及汞化合物之基本物理性質(Schuster, 1991; Schroeder et al., 1991; Lide, 1995)...............................................................................................................................16
表2.9 元素汞與氧化汞之特性比較(Swain, 1997).......................................................17
表2.10 氣相元素汞與氧化性氣體之可能反應與反應速率常數模擬推估................17
表2.11 台灣南部垃圾資源回收(焚化)廠粉狀活性碳採購規格(袁中新，2003).......30
表2.12 物理吸附與化學吸附之差異性(Ruthven, 1984)..............................................32
表2.13 常見之等溫吸附模式(Dastgheib and Rockstraw, 2002；陳威錦，2004).......39
表3.1 原料種類與來源..................................................................................................48
表3.2 商業活性碳之基本物理化學性質......................................................................49
表4.1 起始原料之基本性質分析(n=3).........................................................................62
表4.2 廢棄生質與商用活性碳之各項分析數據(n=3).................................................63
表4.3 廢棄生質與商用活性碳之元素分析結果..........................................................80
表4.4 微區C1s峰值解析之碳氫氧官能基(Series RH)..................................................82
表4.5 微區C1s峰值解析之碳氫氧官能基(Series W)....................................................83
表4.6 微區C1s峰值解析之碳氫氧官能基(Series CAC)...............................................84
表4.7 微區S2p峰值解析之表面官能基(Series RH)......................................................88
表4.8 微區S2p峰值解析之表面官能基(Series W)........................................................89
表4.9 微區S2p峰值解析之表面官能基(Series CAC)....................................................89
表4.10 廢棄生質與商用活性碳之Hg0吸附實驗結果彙整表......................................94
表4.11 選擇用於探討反應動力之廢棄生質與商用活性碳Hg0吸附實驗結果彙整..97
表4.12 擬一階、擬二階吸附動力模式及Elovich equation模擬活性碳吸附Hg0蒸氣之速率常數與相關係數............................................................................................103 vii
圖目錄
圖2.1 所示燃煤過程中汞可能反應途徑及產物種類(Galbreath and Zygarlicke, 2000)........................................................................................................................................10
圖2.2 環境中含汞物種間之化學循環轉換途徑(潘子明，1993)...............................18
圖2.3 活性碳微結構示意圖(Bansal et al., 1988)..........................................................21
圖2.4 活性碳表面可能含氧官能基分佈示意圖..........................................................23
圖2.5 活性碳表面可能含氧酸性官能基(Boehm, 1994)..............................................25
圖2.6 活性碳表面可能含氧鹼性官能基(Boehm, 1994)..............................................25
圖2.7 不同溫度範圍的主要吸附現象(江右君，1999)...............................................33
圖2.8 根據IUPAC分類歸納出來的六類等溫吸附線示意圖。橫軸是氣體相對壓力(Ps/P0)，縱軸為吸附量。(Gregg et al., 1982)..............................................................35
圖2.9 de Boer的Hysteresis loop分類(de Boer, 1958).....................................................36
圖2.10 IUPAC建議的Hysteresis loop分類(江右君，1999)..........................................36
圖2.11 等溫吸附曲線之示意圖例................................................................................38
圖3.1 實驗步驟流程圖..................................................................................................48
圖3.2 活性碳製程設備..................................................................................................49
圖3.3 比表面積分析儀示意圖(Beckman Coulter SA3100).........................................50
圖3.4 汞蒸氣吸附裝置示意圖 (修改自Carey et al., 1998)........................................52
圖3.5 標準氣體產生器..................................................................................................53
圖3.6 元素汞滲透管......................................................................................................53
圖3.7 浮子流量計..........................................................................................................53
圖3.8 固定吸附床..........................................................................................................55
圖3.9 衝擊瓶..................................................................................................................55
圖3.10 去水氣裝置........................................................................................................55
圖3.11 電磁閥控制/數位輸出入模組...........................................................................55
圖3.12 活性碳合成溫度曲線........................................................................................57
圖3.13 吸附實驗流程圖................................................................................................59
圖4.1 活性碳經硫含浸表面改質前後之BET比表面積與孔體積之關係圖.............64
圖4.2 稻殼(Series RH)活性碳之77K N2等溫吸附/脫附曲線.....................................65
圖4.3 產氫廢麥粕(Series W)活性碳之77K N2等溫吸附/脫附曲線...........................66
圖4.4 商用(Series CAC)活性碳之77K N2等溫吸附/脫附曲線..................................67
圖4.5 不同硫含浸溫度對稻殼活性碳(Series RH)之BJH孔徑分佈影響..................71
圖4.6 不同硫含浸溫度對產氫廢麥粕活性碳(Series W)之BJH孔徑分佈影響........71
圖4.7 不同硫含浸溫度對商用活性碳(Series CAC)之BJH孔徑分佈影響...............72
圖4.8 不同硫含浸溫度對稻殼活性碳(Series RH)之微孔孔徑分佈影響...................72
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圖4.9 不同硫含浸溫度對產氫廢麥粕活性碳(Series W)之微孔孔徑分佈影響.........73
圖4.10 不同硫含浸溫度對商用活性碳(Series CAC)之微孔孔徑分佈影響..............73
圖4.11 稻殼活性碳(Series RH)之SEM檢視圖...........................................................75
圖4.12 產氫廢麥粕活性碳(Series W)之SEM檢視圖.................................................76
圖4.13 商用活性碳(Series CAC)之SEM檢視圖........................................................77
圖4.14 稻殼(Series RH)活性碳之元素分析結果.........................................................78
圖4.15 產氫廢麥粕(Series W)活性碳之元素分析結果...............................................79
圖4.16 商用(Series CAC)活性碳之元素分析結果......................................................79
圖4.17 產氫廢麥粕(W)活性碳之XPS全區掃描結果................................................81
圖4.18 硫含浸產氫廢麥粕(W-300S)活性碳之XPS全區掃描結果...........................81
圖4.19 微區C1s峰值解析之碳氫氧官能基含量變化(Series RH)................................85
圖4.20 微區C1s峰值解析之碳氫氧官能基含量變化(Series W)..................................86
圖4.21 微區C1s峰值解析之碳氫氧官能基含量變化(Series CAC).............................86
圖4.22 微區S2p峰值解析之硫官能基含量變化(Series RH)........................................90
圖4.23 微區S2p峰值解析之硫官能基含量變化(Series W)..........................................90
圖4.24 微區S2p峰值解析之硫官能基含量變化(Series CAC)......................................91
圖4.25 Hg0進流量與峰值之檢量線...............................................................................92
圖4.26 廢棄生質與商用活性碳之Hg0吸附實驗結果..................................................95
圖4.27 稻殼(Series RH)活性碳於Hg0蒸氣之吸附貫穿曲線.......................................98
圖4.28 產氫廢麥粕(Series W)活性碳於Hg0蒸氣之吸附貫穿曲線.............................98
圖4.29 商用(Series CAC)活性碳於Hg0蒸氣之吸附貫穿曲線....................................99
圖4.30 稻殼(Series RH)活性碳於Hg0蒸氣之累積吸附曲線.....................................102
圖4.31 產氫廢麥粕(Series W)活性碳於Hg0蒸氣之累積吸附曲線...........................102
圖4.32 商用(Series CAC)活性碳於Hg0蒸氣之累積吸附曲......................................103
圖4.33 擬一階及擬二階吸附動力模式模擬值與RH活性碳吸附Hg0蒸氣實驗值之比較............................................................................................................................105
圖4.34 擬一階及擬二階吸附動力模式模擬值與RH-300S活性碳吸附Hg0蒸氣實驗值之比較....................................................................................................................105
圖4.35 擬一階及擬二階吸附動力模式模擬值與RH-400S活性碳吸附Hg0蒸氣實驗值之比較....................................................................................................................106
圖4.36 擬一階及擬二階吸附動力模式模擬值與RH-650S活性碳吸附Hg0蒸氣實驗值之比較....................................................................................................................106
圖4.37 擬一階及擬二階吸附動力模式模擬值與W活性碳吸附Hg0蒸氣實驗值之比較............................................................................................................................107
圖4.38 擬一階及擬二階吸附動力模式模擬值與W-300S活性碳吸附Hg0蒸氣實驗值之比較....................................................................................................................107
ix
圖4.39 擬一階及擬二階吸附動力模式模擬值與W-400S活性碳吸附Hg0蒸氣實驗值之比較....................................................................................................................108
圖4.40 擬一階及擬二階吸附動力模式模擬值與W-650S活性碳吸附Hg0蒸氣實驗值之比較....................................................................................................................108
圖4.41 擬一階及擬二階吸附動力模式模擬值與CAC活性碳吸附Hg0蒸氣實驗值之比較........................................................................................................................109
圖4.42 擬一階及擬二階吸附動力模式模擬值與CAC-300S活性碳吸附Hg0蒸氣實驗值之比較................................................................................................................109
圖4.43 擬一階及擬二階吸附動力模式模擬值與CAC-400S活性碳吸附Hg0蒸氣實驗值之比較................................................................................................................110
圖4.44 擬一階及擬二階吸附動力模式模擬值與CAC-650S活性碳吸附Hg0蒸氣實驗值之比較................................................................................................................110
圖4.45 稻殼活性碳(RH)套用孔隙擴散模式之趨勢圖..............................................114
圖4.46 硫含浸稻殼活性碳(RH-300S)套用孔隙擴散模式之趨勢圖........................114
圖4.47 硫含浸稻殼活性碳(RH-400S)套用孔隙擴散模式之趨勢圖........................115
圖4.48 硫含浸稻殼活性碳(RH-650S)套用孔隙擴散模式之趨勢圖........................115
圖4.49 產氫廢麥粕活性碳(W)套用孔隙擴散模式之趨勢圖....................................116
圖4.50 硫含浸產氫廢麥粕活性碳(W-300S)套用孔隙擴散模式之趨勢圖..............116
圖4.51 硫含浸產氫廢麥粕活性碳(W-400S)套用孔隙擴散模式之趨勢圖..............117
圖4.52 硫含浸產氫廢麥粕活性碳(W-650S)套用孔隙擴散模式之趨勢圖..............117
圖4.53 商用活性碳(CAC)套用孔隙擴散模式之趨勢圖...........................................118
圖4.54 硫含浸商用活性碳(CAC-300S)套用孔隙擴散模式之趨勢圖......................118
圖4.55 硫含浸商用活性碳(CAC-400S)套用孔隙擴散模式之趨勢圖......................119
圖4.56 硫含浸商用活性碳(CAC-650S)套用孔隙擴散模式之趨勢圖......................119

參
Aha Kinetics of Adsorption and Desorption and the Elovich
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