臺灣博碩士論文加值系統

本研究以甲烷作為低溫電漿重組產氫氣的原料，探討不同射頻電源輸出功率、N2/CH4進氣比例等參數對甲烷轉換率(〖Conv.〗_(〖CH〗_4 ))及氫氣生成體積百分比(V_(H_2 )%)之影響。實驗結果顯示利用氮氣電漿之高能量電子，打斷甲烷之鍵結，當RF輸入功率為125 W、N2/CH4流速比為8/24時為最佳參數且尚未添加觸媒情況下，甲烷轉換率達70%且氫氣產率50%，並針對此電漿環境做溫度量測，當輸入125 W功率且經重組反應一小時後，電漿環境溫度在58oC。為了提高重組反應的效益，選以活性碳布(Activity carbon paper，AC)及導電碳布(Conductive carbon paper，CC)作為觸媒來輔助，實驗結果顯示，碳布觸媒配合重組反應可增加氫氣生成體積百分比及甲烷轉換率。添加導電碳布在低溫電漿甲烷重組反應中氫氣生成所提升效果達20%；甲烷轉換率增加了19%。此外，重組反應過程中所產生的殘碳並不會影響到碳觸媒在電漿重組反應中的表現，相較於傳統高耗能高溫裂解甲烷產氫氣，本系統具高產率高轉換率之優點。

Methane reforming has been carried out by low temperature radio frequency (RF) plasma. The plasma was composed of mixture gas with different N2/CH4 flow ratios. In order to obtain optimal condition, several parameters, including RF powers and ratio of N2/CH4 flow rates were used to achieve the maximal yield of hydrogen and conversion of methane. The results indicate that 125 W of RF power under N2/CH4 flow rate of 8/24 showed 70% methane conversion rate and 50% hydrogen production yield without carbon catalyst. Temperature measuring of radio frequency plasma reactor which indicates 58oC with 125 W for a hour operation. Adding conductive carbon cloth (CC) and active carbon cloth (AC) can be the catalyst to enhance reforming efficiency. Through the analytic results of ICR and Raman, conductive carbon cloth has performance of higher conductivity and degree of graphitization than active carbon cloth. Therefore, hydrogen production yield increased from 50% to 56% and 60% when the AC and CC used. Conversion rate of CH4 increased from 70% to 78% and 84% as AC and CC. In comparison with CC, AC and without catalyst, CC has higher hydrogen production yield and higher conversion rate of CH4 than AC and without catalyst added.

誌謝 I
摘要 III
Abstract IV
圖目錄 VII
表目錄 XI
第一章 緒論 1
1-1前言 1
1-2研究動機 3
第二章 文獻回顧 5
2-1 氫能源 5
2-1-1 氫能源簡介 5
2-1-2 氫氣生產技術 6
2-2 電漿技術簡介 12
2-2-1 電漿基本原理 12
2-2-2 應用於重組反應之電漿類型 19
2-3-1電漿裂解甲烷重組產氫 27
2-3-2甲烷電漿輔助觸媒重組產氫 31
2-3-3 碳觸媒 33
第三章 實驗方法 36
3-1實驗設計與方法 36
3-1-1 實驗材料 36
3-1-2 實驗設備 37
3-1-3 實驗流程 38
3-2電漿重組反應 41
3-2-1 甲烷電漿重組反應 41
3-2-2 碳觸媒輔助甲烷電漿重組產氫 42
3-2-3 I-V曲線之電子溫度 43
3-2-4 實驗參數代碼 46
3-3 甲烷電漿重組系統之環境溫度量測 47
3-4分析儀器 48
3-4-1氣相層析儀(GC-TCD) 48
3-4-2冷場發射式掃描電子顯微鏡(FESEM) 50
3-4-3拉曼光譜儀(Raman) 51
3-4-4穿透阻抗量測(ICR) 54
3-4-5高解析比表面積分析儀(BET) 55
第四章 結果與討論 58
4-1 甲烷電漿重組 58
4-1-1 N2/CH4進氣比例 58
4-1-2射頻功率 60
4-1-3 N2/CH4 總進氣量 61
4-1-4甲烷電漿環境溫度量測 63
4-1-5 CH4殘碳之分析 64
4-1-5-1 冷場發射式電子顯微鏡 64
4-1-5-2拉曼光譜儀 66
4-1-5-3殘碳對電漿重組反應的影響 68
4-2 活性碳布與導電碳布之材料分析 70
4-2-1 高解析比表面積分析 70
4-2-2 拉曼光譜 72
4-2-3 穿透阻抗量測 74
4-3 碳觸媒輔助甲烷電漿重組反應 75
4-3-1 氣相組成 75
4-3-2 活化能 78
4-3-2 自偏壓(self-bias) 80
4-3-3 I-V curve 84
4-3-4 重組反應後之碳觸媒分析 86
4-3-4-1 拉曼光譜儀 86
4-3-4-2 穿透阻抗量測 88
4-3-5 碳觸媒產氫穩定性測試 89
第五章 結論 91
參考文獻 93

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