臺灣博碩士論文加值系統

本研究利用微波來促進纖維物質(柳杉、稻稈、蔗渣)酸水解，分別探討一階段及二階段(先經鹼處理)水解之最適操作條件，隨後再以最佳水解條件所得水解液進行批次醱酵產氫試驗。
在一階段微波水解中，柳杉最佳水解條件為以0.49%硫酸(pH 1.0)進行操作，在固/液比15/100、溫度180℃維持20 min、以及添加氯化鈉7 g/l之條件下，獲致總糖及還原糖產率分別為0.227及0.226 g/g cryptomeria。稻稈最佳水解條件為以0.49%硫酸(pH 1.0)進行操作，在固/液比15/100、溫度180℃維持5 min、以及不添加氯化鈉之條件下，獲致總糖及還原糖產率分別為0.334及0.332 g/g rice straw。蔗渣最佳水解條件為以0.49%硫酸(pH 1.0)進行操作，在固/液比10/100、溫度150℃維持20 min、以及不添加氯化鈉之條件下，獲致總糖及還原糖產率分別為0.409及0.385 g/g bagasse。
在二階段微波水解中，柳杉先以0.2% NaOH進行微波前處理(固/液比15/100，180℃，30 min)，而後再進行微波硫酸水解(固/液比10/100，180℃，20 min)，獲致總糖及還原糖產率分別為0.255及0.220 g/g cryptomeria。稻稈鹼處理後再進行微波硫酸水解(固/液比10/100，180 ℃，5 min)，獲致總糖及還原糖產率分別為0.320及0.319 g/g rice straw。
在醱酵產氫試驗方面，一階段微波酸水解液經過量鹼處理後均可有效轉化成氫氣。其中柳杉及蔗渣以磷酸水解液可獲致最大氫氣產率，分別為5.22及4.91 mmol H2/g total sugar。而稻稈以鹽酸水解液可獲致最大氫氣產率4.02 mmol H2/g total sugar。在二階段微波酸水解液醱酵產氫試驗中，經過量鹼處理之柳杉及稻稈之水解液，其氫氣產率分別為5.56及5.51 mmol H2/g total sugar。

In this study, the microwave irradiation was used to promote the hydrolysis of cellulosic material (cryptomeria, rice straw, and bagasse) in various acid solutions (hydrochloric acid, sulfuric acid, phosphoric acid). One- and two-stage (preatreatment with alkaline solution) hydrolyses were investigated to obtain the optimal operation condition. Sequentially, the hydrolysate obtained under the optimum conditions was used as the feedstock to produce H2 in a batch experiment.
For one-stage microwave hydrolysis, the optimum hydrolysis conditions for cryptomeria were 0.49% sulfuric acid (pH 1.0) at a solid/liquid ratio of 15/100, 180℃ for 20 min, and addition of 7 g/l NaCl. The yields of total sugar and reducing sugar were 0.227 and 0.226 g/g cryptomeria, respectively. For rice straw, the optimum hydrolysis conditions were 0.49% sulfuric acid at a solid/liquid ratio of 15/100, 180℃ for 5 min, and without NaCl addition. The yields of total sugar and reducing sugar were 0.334 and 0.332 g/g rice straw, respectively. The optimum hydrolysis conditions for bagasse were 0.49% sulfuric acid at a solid/liquid ratio of 10/100, 150℃ for 20 min, and without NaCl addition. The yields of total sugar and reducing sugar were 0.409 and 0.385 g/g bagasse, respectively.
For two-stage microwave hydrolysis, cryptomeria was pretreated using microwave irradiation (solid/liquid ratio 15/100 and 180℃ for 30 min) in 0.2% NaOH solution; afterward the pretreated cryptomeria proceeded microwave sulfuric acid hydrolysis (solid/liquid ratio 10/100 and 180℃ for 20 min). The results showed that the yields of total sugar and reducing sugar were 0.255 and 0.220 g/g cryptomeria, respectively. For rice straw, the yields of total sugar and reducing sugar were 0.320 and 0.319 g/g rice straw, respectively, with two-stage microwave hydrolysis (in H2SO4 solution, solid/liquid ratio 10/100, and 180℃ for 5 min).
In biohydrogen production experiment, hydrolysate from one-stage microwave-acid hydrolysis via overliming treatment could be transform into hydrogen efficiently. The hydrolysates of cryptomeria and bagasse with phosphoric acid hydrolysis obtained the maximum hydrogen yield of 5.22 and 4.91 mmol H2/g total sugar, respectively. For rice straw, the hydrolysate with hydrochloric acid hydrolysis got the maximum hydrogen yield of 4.02 mmol H2/g total sugar. For hydrogen production from hydrolysate with two-stage microwave-acid hydrolysis and overliming treatment, cryptomeria and rice straw hydrolysates gained a yield of 5.51 and 5.56 mmol H2/g total sugar, respectively.

摘要 I
Abstract II
目錄 IV
圖目錄 VIII
表目錄 XI
第一章 緒論 1
1-1 前言 1
1-2 研究動機及目的 2
1-3 實驗架構 2
第二章 原理與文獻回顧 4
2-1 生質能源 4
2-2 木質纖維素 4
2-2-1 纖維素 4
2-2-2 半纖維素 6
2-2-3 木質素 8
2-3 微波 8
2-3-1 微波加熱原理 8
2-3-2 微波加熱與傳統加熱法之比較 9
2-3-3 微波技術的應用 10
2-4 纖維物質水解 12
2-4-1 化學方法 12
2-4-1-1 濃酸水解 12
2-4-1-2 稀酸水解 12
2-4-2 物理方法 12
2-4-2-1 蒸氣爆破 12
2-4-2-2 水熱法 13
2-4-2-3 氨水前處理 13
2-4-3 酵素水解 14
2-4-3-1 內切型纖維素分解酵素 14
2-4-3-2 外切型纖維素分解酵素 14
2-4-3-3 β-葡萄糖酵素(β-glucosidase) 15
2-4-4 聚木糖酵素水解 15
2-4-4-1 Endo-β-1,4-xylanase (E.C.3.2.1.8) 15
2-4-4-2 β-1,4-xylosidase (E.C.3.2.1.37) 15
2-4-4-3 α-L-Arabinofuranosidases (E.C.3.2.1.55) 15
2-4-4-4 α-D-Glucuronidase (E.C.3.2.1.1) 16
2-4-4-5 Acetylxylan esterase (E.C.3.1.1.6)和Phenolic acid esterases 16
2-5 酸水解副產物去除方法 16
2-5-1 醱酵抑制因子 16
2-5-1-1 糠醛和羥甲基糠醛的抑制作用 16
2-5-1-2 乙酸的抑制作用 18
2-5-1-3 木質素降解產物 18
2-5-2 抑制物去除方法 19
2-5-2-1 物理方法 19
2-5-2-2 化學方法 20
2-5-2-3 生物方法 21
2-5-2-4 混合方法 21
2-6 厭氧污泥發酵產氫 22
2-6-1 厭氧產氫微生物特性 25
2-6-2 Clostridium之特性 26
2-6-3 厭氧醱酵之環境因子 28
2-6-3-1 溫度 28
2-6-3-2 pH 28
2-6-3-3 營養鹽 28
2-6-3-4 毒性物質 32
2-6-3-5 攪拌之影響 34
2-6-3-6 基質與產物濃度 34
2-6-3-7 ORP 35
2-6-3-8 氫分壓 35
2-6-3-9 氫氣產率(yield) 35
2-6-4 厭氧醱酵代謝途徑 36
2-6-4-1 葡萄糖厭氧醱酵途徑 36
2-6-4-2 木糖的醱酵途徑 37
2-7 Gompertz修正模式 39
2-8 文獻回顧 39
第三章 實驗材料及方法 44
3-1 藥品試劑與培養基 44
3-1-1 碳源 44
3-1-2 緩衝鹽類 44
3-1-3 無機鹽類 44
3-1-4 其他 44
3-2 分析儀器及方法 45
3-2-1 氣體組成分析 45
3-2-2 液體組成分析 46
3-2-3 菌量分析 46
3-2-4 總糖分析 46
3-2-5 還原糖分析 47
3-3 纖維物質微波酸水解實驗裝置與方法 48
3-3-1 實驗裝置 48
3-3-2 不同酸濃度與氯化鈉濃度微波水解試驗 49
3-3-2-1 不同鹽酸濃度微波水解試驗試驗 49
3-3-2-2 不同氯化鈉濃度微波水解試驗 49
3-3-3 一階段微波酸水解 49
3-3-3-1 柳杉微波酸水解 49
3-3-3-2 稻稈微波酸水解 50
3-3-3-3 蔗渣微波酸水解 52
3-3-4 二階段微波酸水解 53
3-3-4-1 以不同氫氧化鈉濃度進行柳杉微波前處理 53
3-3-4-2 以不同氫氧化鈉濃度進行稻稈微波前處理 54
3-3-5 水解產率 54
3-4 批次產氫實驗裝置與方法 54
3-4-1 儀器裝置 54
3-4-2 產氫菌來源 55
3-4-3 培養基濃度 55
3-4-4 纖維物質直接醱酵產氫實驗 56
3-4-5 水解液直接醱酵產氫實驗 56
3-4-6 水解液經過量鹼處理醱酵產氫實驗 57
3-4-7 修正型Gompertz Model模式探討 57
3-4-8 氫氣產率 (yield) 58
第四章 結果與討論 59
4-1 酸與氯化鈉濃度對微波水解之影響 59
4-1-1 不同鹽酸濃度對微波水解之影響 59
4-1-2 不同氯化鈉濃度對微波水解之影響 61
4-2 一階段微波酸水解實驗 61
4-2-1 柳杉之不同酸液微波水解實驗 62
4-2-1-1 以鹽酸水解實驗 62
4-2-1-2 以硫酸水解實驗 66
4-2-1-3 以磷酸水解實驗 70
4-2-1-4 柳杉之不同酸水解效率評比 74
4-2-2 稻稈不同酸微波水解實驗 75
4-2-2-1 以鹽酸水解實驗 75
4-2-2-2 以硫酸水解實驗 79
4-2-2-3 以磷酸水解實驗 83
4-2-2-4 稻桿之不同酸水解效率評比 87
4-2-3 蔗渣不同酸微波水解實驗 88
4-2-3-1 以鹽酸水解實驗 88
4-2-3-2 以硫酸水解實驗 92
4-2-3-3 以磷酸水解實驗 96
4-2-3-4 蔗渣之不同酸水解效率評比 100
4-3 二階段微波酸水解實驗 101
4-3-1 以不同氫氧化鈉濃度進行柳杉微波前處理 102
4-3-1-1 鹼處理後以固/液比15/100進行硫酸水解 102
4-3-1-2 鹼處理後以固/液比10/100進行硫酸水解 103
4-3-2 以不同氫氧化鈉濃度進行稻稈微波前處理 104
4-3-2-1 鹼處理後以固/液比15/100進行硫酸水解 104
4-3-2-2 鹼處理後以固/液比10/100進行硫酸水解 105
4-3-3 一階段與二階段微波水解效率評比 107
4-4 纖維物質一階段微波水解液批次產氫實驗 108
4-4-1 葡萄糖與木糖醱酵產氫實驗 108
4-4-2 纖維物質直接醱酵產氫實驗 110
4-4-3 纖維物質水解液直接醱酵產氫實驗 111
4-4-3-1 柳杉水解液直接醱酵產氫實驗 111
4-4-3-2 稻稈水解液直接醱酵產氫實驗 114
4-4-3-3 蔗渣水解液直接醱酵產氫實驗 116
4-4-4 纖維物質水解液經過量鹼處理後再行醱酵產氫 119
4-4-4-1 柳杉水解液醱酵產氫實驗 120
4-4-4-2 稻稈水解液醱酵產氫實驗 123
4-4-4-3 蔗渣水解液醱酵產氫實驗 125
4-4-5 水解液未處理與經鹼處理之產氫效率評比 128
4-5 纖維物質二階段微波水解液批次產氫實驗 129
4-5-1 水解液直接醱酵產氫 129
4-5-2 水解液經過量鹼處理後再行醱酵產氫 130
4-5-3 一階段與二階段微波水解液之產氫效率評比 132
第五章 結 論 134
參考文獻 137
附錄一 146
附錄二 150
附錄三 154
附錄四 157
致 謝 163

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