臺灣博碩士論文加值系統

現今工業革命造成生活便利及發達後，卻也發生許多令人隱憂的問題產生，燃燒石化原料產生的氣體日益影響著全世界的氣候，例如：甲烷及二氧化碳。本研究即是將甲烷溫室氣體利用高溫的反應將其轉換為氫氣。
觸媒則以逆滴定沉澱法製備鎳鈰中孔洞觸媒，在利用含浸法將觸媒披覆於蜂巢擔體。並使用感應耦合電漿光譜儀(ICP)、掃描式電子顯微鏡(VVSEM)、多功能薄膜X光繞射儀(XRD)，示差掃描熱量-熱重分析聯用儀(SDT)、程溫還原分析(TPR)分別進行觸媒特性分析。甲烷水蒸氣重組實驗則以溫度、WHSV、進料的水碳莫耳比，甲烷乾重組實驗則以溫度、WHSV不同的實驗參數設定藉以尋找甲烷重組最佳反應條件及結果。
實驗結果顯示，自製的觸媒披覆於蜂巢結構，對於甲烷重組有良好的活性，蜂巢反應器應用於甲烷重組的效果也優於傳統的填充床反應器。在於兩種重組法反應，反應溫度為高溫的情況下，甲烷轉化率都可到達85%以上、二氧化碳轉化率都可達到75%。氫氣為主要產氣，產率及選擇率都高於80%以上。

In these days revolution makes life convenient and well-developed, but it cause lots of worries problems, burning fossil fuel produce greenhouse gases polluted the environment of the whole world, such as methane and carbon dioxide. In this study using methane greenhouse gases with high temperature reforming convert into hydrogen.
Catalyst prepared by using reverse precipitation method, than use impregnation method to coat catalyst on honeycomb. Catalyst characterization with ICP,VVSEM,XRD,SDT,TPR. Methane steam reforming by changing reaction temperature, WHSV, water carbon ratio, Methane dry reforming by changing reaction temperature, WHSV to find the best reaction factor and result.
Experimental results show that catalyst coating on honeycomb has a good activity in methane reforming better than traditional packed bed reactor. In two kinds of reforming reaction temperature at high level methane conversion is higher than 85%, carbon dioxide is about 78%, Hydrogen is the main syngas the yield and s selectivity are higher than 80%.
keyword：honeycomb、Ni/CeO2、methane steam reforming、methane dry reforming

誌 謝 I
摘 要 II
ABSTRACT III
目 錄 IV
圖目錄 IX
表目錄 XII
第一章 緒論 1
1-1 前言 1
1-2 研究目的 3
第二章 文獻回顧 4
2-1 蜂巢結構 4
2-1-1 蜂巢結構介紹 4
2-1-2 蜂巢結構應用 5
2-1-2-1 機械性應用 6
2-1-2-2 化學性應用 8
2-2 氫能介紹 12
2-2-1 產氫方式 13
2-2-1-1 水電解法 13
2-2-1-2 光電解法 13
2-2-1-3 電漿重組法 14
2-2-1-4 生物法 14
2-2-1-5 熱化學法 15
2-2-1-6 蒸氣重組法 16
2-3 甲烷重組 17
2-3-1 甲烷二氧化碳重組 17
2-3-2 甲烷水蒸氣重組 18
2-3-3 部分氧化重組反應 19
2-3-4 自熱化重組反應 20
2-4 觸媒 21
2-4-1 觸媒介紹 21
2-4-1-1 擔體 22
2-4-1-2 活性載體 22
2-4-1-3 改質劑 24
2-4-2觸媒製備 26
2-4-2-1 共沉澱法(Co-precipitation) 26
2-4-2-2 含浸法(Impregnation) 27
2-4-2-3 溶膠凝膠法(Sol-gel method) 28
2-4-2-4 無電鍍法（Electroless plating） 28
第三章 實驗方法與實驗流程 36
3-1 實驗目的及方法 36
3-1-1 實驗目的 36
3-1-2 實驗方法 36
3-2 實驗規劃 37
3-3 共沉澱法製備觸媒 38
3-4 基材前處理 41
3-5 含浸法製備蜂巢結構觸媒 43
3-6 重組反應 45
第四章 結果討論 49
4-1 觸媒特性分析 49
4-1-1 示差掃描量熱-熱重分析 49
4-1-2 觸媒表面形態分析 51
4-1-3 成分分析 53
4-1-4 觸媒微結構分析 54
4-1-5 還原溫度檢測 55
4-2 甲烷重組 58
4-2-1 實驗參數討論 58
4-2-2 空白實驗 60
4-2-3 蜂巢與填充床反應器實驗比較 61
4-2-4 甲烷水蒸氣重組 63
4-2-4-1 不同溫度下甲烷水蒸氣重組之結果 63
4-2-4-2 不同水碳比下甲烷水蒸氣重組之結果 64
4-2-4-3 不同WHSV下甲烷水蒸氣重組之結果 65
4-2-5 甲烷二氧化碳重組 72
4-2-5-1 不同溫度下甲烷乾重組之結果 72
4-2-5-2 不同WHSV下甲烷乾重組之結果 73
4-2-5-3 合成氣之討論 74
4-2-6 反應曲面分析法 79
4-2-6-1 甲烷水蒸氣重組之反應曲面分析結果 79
4-2-6-2 甲烷二氧化碳重組之反應曲面分析結果 80
第五章 結論與展望 85
5-1 結論 85
5-2 展望 86
附錄 87
附錄A： 實驗化學藥品與儀器 87
附錄A-1： 實驗化學藥品 87
附錄A-2： 實驗儀器 89
附錄A-3： 實驗所使用的氣體 90
附錄A-4： 藥品供應商資料 91
附錄B： 分析設備及方法 92
附錄B-1： 示差掃描熱量-熱重分析聯用儀 92
附錄B-2： 感應耦合電漿光譜儀 94
附錄B-3： 可變真空掃描式電子顯微鏡及能量散佈儀 96
附錄B-4： 多功能薄膜X光繞射儀 98
附錄B-5： 程溫還原分析 100
附錄B-6： 氣相色層分析儀 102
參考文獻 103

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