探討添加油茶果殼生物碳於兩階段乾式厭氧發酵來轉換菇包木屑為氫氣與甲烷之研究

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王竹萱(Chu-Hsuan Wang) 查詢紙本館藏

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論文名稱

探討添加油茶果殼生物碳於兩階段乾式厭氧發酵來轉換菇包木屑為氫氣與甲烷之研究
(Study on hydrogen and methane of spent mushroom substrate in two-stage dry anaerobic fermentation by adding Camellia oleifera shell biochar)

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至系統瀏覽論文 (2028-7-20以後開放)

摘要(中)

隨著全球對能源需求的增加，開發生質能源已成為當今重要課題，厭氧發酵是利用微生物在無氧環境下將廢棄物轉換為沼氣的技術。在台灣，每年產生超過150萬噸的菇類和20萬噸的廢棄太空包，而這些菇包木屑通常以野外焚燒或堆置方式處理，造成環境汙染。然而，菇包木屑中的纖維素可以進行厭氧發酵，產生沼氣用於工業發電，達到廢棄物轉換為生質能源的循環經濟目的。厭氧發酵中菌落所適合的環境大不相同，因此本研究開發兩階段式反應器，使不同菌落在合適的環境下生長，解決微生物間互相抑制問題，分別為1st-stage 酸化/產氫氣製程，發酵溫度35°C、起始pH5.5，2nd-stage甲烷化/產甲烷製程，發酵溫度50°C，來改善傳統單階段發酵穩定性不足之缺點。
菇包木屑中碳含量較高，但若直接投入厭氧發酵中會造成碳氮比失衡，抑制產酸菌及產甲烷菌的活性，因此本研究透過共消化建立最佳碳氮比，並選用畜牧業廢棄物為氮源(如: 雞糞、尿素及雞羽毛等)來解決系統營養源不足問題，本研究結果顯示選用雞糞作為氮源可獲得最高揮發性脂肪酸(Volatile Fatty Acid ,VFA)濃度25.1g/L及氫氣和甲烷產量分別為151mL及370mL，為三組氮源中產氫產甲烷效率最高。
本研究同時開發乾式厭氧發酵來提高廢棄物處理之含量，乾式厭氧發酵所需反應體積較低，可減少人力及時間成本，缺點為會有過多抑制物的累積，及產甲烷時間滯後和產率降低等問題。本研究透過添加油茶果殼生物碳(Camellia Oleifera Shell Biochar ,COSBC)於厭氧發酵系統中，並且探討油茶果殼生物碳最佳製備參數，如熱裂解溫度及時間以尋求最適化製程，其中發現在1st-stage 酸化/產氫氣製程中以COSBC 700°C,1HR有最高VFA濃度可高達28.8 g/L，氨氮抑制物下降21.2%，累積氫氣產量提高72.2%。最後探討COSBC添加量對第一階段影響，當添加量提高至20%時，VFA濃度提升至31.1 g/L，氨氮抑制物下降33.9%，累積氫氣產量提高106.6%。將條件COSBC 700°C,1HR,1.5g、3.0及4.5g投入2nd-stage中，發現COSBC 4.5g可提高25.1%甲烷產量，氨氮濃度下降44.9%，甲烷含量約佔42-71%。綜合以上厭氧發酵因素，觀察到COSBC的添加可加速酸化/產氫氣階段VFA的產生，在產甲烷化階段加速VFA降解，解決產甲烷滯後問題，提供緩衝能力及鹼度使發酵系統中抑制物降低來提升整體沼氣產量，以解決高固體濃度下所遇問題，提高了兩階段厭氧發酵之效率。

摘要(英)

With the increasing global energy demand, the development of sustainable energy sources has become a crucial task. Anaerobic fermentation, a microbial process that converts waste into biogas in an oxygen-deprived environment, holds promise for addressing this challenge. In Taiwan, large quantities of spent mushroom substrate (SMS) and waste space bags are generated annually, posing environmental pollution issues when disposed of through incineration or landfilling. However, the cellulose-rich SMS can undergo anaerobic digestion to produce biogas for industrial power generation, promoting the conversion of waste into bioenergy within a circular economy framework.
To optimize the fermentation process, a two-stage reactor system was developed to accommodate different microbial communities and alleviate microbial inhibition. The first stage involved acidogenesis and hydrogen production at 35°C and pH 5.5, while the second stage focused on methanogenesis at 50°C. This approach aimed to overcome stability issues observed in traditional single-stage fermentation.The carbon-to-nitrogen ratio imbalance in SMS hampers fermentation by inhibiting acidogenic and methanogenic bacteria. To address this, co-digestion strategies incorporating livestock waste as a nitrogen source (e.g., chicken manure, urea, and chicken feathers) were investigated. Results demonstrated that using chicken manure as a nitrogen source achieved the highest volatile fatty acid (VFA) concentration of 25.1 g/L, along with hydrogen and methane yields of 151 mL and 370 mL, respectively, outperforming other nitrogen sources.
Furthermore, dry anaerobic fermentation was employed to increase waste treatment capacity, reducing labor and time requirements. However, challenges such as inhibitory substance accumulation and reduced methane production were observed. This study addressed these issues by adding Camellia Oleifera Shell Biochar (COSBC) to the anaerobic fermentation system and investigated the optimal preparation parameters for COSBC, such as pyrolysis temperature and time, to optimize the process. It was found that in the first stage of acidification/hydrogen production, COSBC prepared at 700°C for 1 hour achieved the highest VFA concentration of up to 28.8 g/L, a 21.2% decrease in ammonia nitrogen inhibitors, and a 72.2% increase in cumulative hydrogen production. The study also examined the effect of COSBC addition on the first stage. When the addition amount was increased to 20%, the VFA concentration increased to 31.1 g/L, the ammonia nitrogen inhibitors decreased by 33.9%, and the cumulative hydrogen production increased by 106.6%. In the second stage, introducing COSBC at dosages of 1.5 g, 3.0 g, and 4.5 g reveals that COSBC 4.5 g results in a 25.1% increase in methane production, a 44.9% decrease in ammonia nitrogen concentration. In conclusion, the two-stage anaerobic fermentation of SMS, combined with nutrient optimization and the use of COSBC, demonstrated improved biogas production. This approach offers a solution for converting high-solid waste into bioenergy efficiently and sustainably.

關鍵字(中)

★ 兩階段厭氧發酵
★ 菇包木屑
★ 生質能源
★ 乾式厭氧發酵
★ 油茶果殼生物碳
★ 雞糞
★ 雞羽毛
★ 尿素

關鍵字(英)

★ Two-stage anaerobic fermentation
★ Spent mushroom substrate
★ bioenergy
★ Dry anaerobic fermentation
★ Camellia oleifera shell biochar
★ Chicken manure
★ Chicken feather
★ Urea

論文目次

摘要 I
ABSTRACT III
致謝 V
目錄 VI
圖目錄 X
表目錄 XIV
一、緒論 1
1-1 研究動機 1
1-2 研究目的 2
二、文獻回顧 4
2-1 厭氧發酵 4
2-1-1 水解(Hydrolysis) 5
2-1-2 揮發性脂肪酸生成(Acidogenic fermentation) 5
2-1-3 氫氣、乙酸生成(Hydrogen-producing Acetogenesis) 5
2-1-4 甲烷生成(Methanogesis) 5
2-2 厭氧發酵因素 6
2-2-1 溫度 6
2-2-2 pH 7
2-2-3 VFA(Volatile fatty acid) 9
2-2-4 碳氮比C/N ratio 9
2-2-5 共發酵(co-digestion) 11
2-3 兩階段厭氧發酵 12
2-4 乾式厭氧發酵 13
2-5 菇包木屑(SMS:SPENT MUSHROOM SUBSTRATE) 15
2-6 氮源選擇 17
2-6-1 雞糞(CM: Chicken Manure) 17
2-6-2 雞羽毛(Chicken Feather) 18
2-6-3 尿素(Urea) 20
2-7 生物碳(BIOCHAR) 21
2-7-1 吸附抑制物 22
2-7-2 緩衝能力 23
2-7-3 電子轉移機制 25
2-8 油茶果殼(CAMELLIA OLEIFERA SHELL, COS) 27
三、材料與方法 29
3-1 實驗規劃 29
3-2 實驗材料 30
3-2-1 太空包菇包木屑(SMS) 30
3-2-2 雞糞(CM) 30
3-2-3 雞羽毛(CF) 30
3-2-4 尿素(UREA) 30
3-2-5 油茶果殼生物碳(COS BC) 31
3-2-6 厭氧汙泥 31
3-3 實驗藥品 32
3-4 實驗儀器與設備 33
3-5 實驗方法 34
3-5-1 生物碳製備方法 34
3-5-2 菇包木屑製備方法 34
3-5-3 產酸汙泥預處理 34
3-5-4 產甲烷汙泥馴養 34
3-5-5 1st-stage process(酸化/產氫製程) 35
3-5-6 2nd-stage process(甲烷化/產甲烷製程) 35
3-5-7 油茶果殼生物碳的pH值與導電度和時間關係 36
3-6 分析方法 37
3-6-1 總固體含量(TS: Total Solid)測量 37
3-6-2 揮發性固體量(VS: Volatile Solid)測量 37
3-6-3 氨氮含量檢測-靛酚比色法 37
3-6-4 沼氣(Biogas)測量 40
3-6-5 沼氣成分測量-氣相層析儀(GC-TCD) 40
3-6-6 發酵液成分測量-(GC-FID) 44
四、結果與討論 47
4-1 最適化氮源探討 47
4-1-1 VFA在1st-stage不同氮源下的變化量 47
4-1-2 VFA組成在1st-stage不同氮源下的變化量 49
4-1-3 NH3-N在1st-stage不同氮源下的變化量 51
4-1-4 Biogas/H2/CH4/CO2在1st-stage不同氮源下的變化量 53
4-1-5 pH在1st-stage不同氮源下的變化量 56
4-1-6 VFA在2nd-stage不同氮源下的變化量 57
4-1-7 NH3-N在2nd-stage不同氮源下的變化量 60
4-1-8 Biogas/H2/CH4/CO2在2nd-stage不同氮源下的變化量 61
4-1-9 pH在2nd-stage不同氮源下的變化量 65
4-2 添加不同熱裂解溫度油茶果殼生物碳於1ST-STAGE的影響 66
4-2-1 VFA在1st-stage不同熱裂解溫度COSBC下的變化量 66
4-2-2 VFA組成在1st-stage不同熱裂解溫度COSBC下的變化量 68
4-2-3 NH3-N在1st-stage不同熱裂解溫度COSBC下的變化量 70
4-2-4 Biogas/H2/CH4/CO2在1st-stage不同熱裂解溫度COSBC下的變化量 72
4-2-5 pH在1st-stage不同熱裂解溫度COSBC下的變化量 76
4-3 添加不同熱裂解時間油茶果殼生物碳於1ST-STAGE的影響 77
4-3-1 VFA在1st-stage不同熱裂解時間COSBC下的變化量 77
4-3-2 VFA組成在1st-stage不同熱裂解時間COSBC下的變化量 79
4-3-3 NH3-N在1st-stage不同熱裂解時間COSBC下的變化量 81
4-3-4 Biogas/H2/CH4/CO2在1st-stage不同熱裂解時間COSBC下的變化量 83
4-3-5 pH在1st-stage不同熱裂解時間COSBC下的變化量 87
4-4 不同添加量油茶果殼生物碳於1ST-STAGE的影響 88
4-4-1 VFA在1st-stage不同添加量COSBC下的變化 88
4-4-2 VFA組成在1st-stage不同添加量COSBC下的變化量 90
4-4-3 NH3-N在1st-stage不同添加量COSBC下的變化量 93
4-4-4 Biogas/H2/CH4/CO2在1st-stage不同添加量COSBC下的變化量 95
4-4-5 pH在1st-stage不同添加量COSBC下的變化量 99
4-5 添加油茶果殼生物碳於2ND-STAGE的影響 100
4-5-1 添加COSBC對2nd-stage VFA 的影響 101
4-5-2 添加COSBC對2nd-stage NH3-N的影響 105
4-5-3 添加COSBC對2nd-stage Biogas/H2/CH4/CO2的影響 107
4-5-4 添加COSBC對2nd-stage pH的影響 111
4-6 時間對油茶果殼生物碳PH與導電度的影響 112
五、結果討論與建議 115
5-1 結果討論 115
5-2 建議 117
六、參考文獻 118

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指導教授

徐敬衡(Chin-Hang Shu)

審核日期

2023-7-20

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