以CuO/SDC觸媒在富氫下行一氧化碳選擇氧化｜國立清華大學博碩士論文庫

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研究生：	林聖欽
論文名稱：	以CuO/SDC觸媒在富氫下行一氧化碳選擇氧化 Selective CO oxidation in rich hydrogen by using CuO/SDC
指導教授：	黃大仁 Ta-Jen Huang
口試委員:
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2001
畢業學年度：	89
語文別：	中文
論文頁數：	84
中文關鍵詞：	導氧離子材料、選擇氧化、一氧化碳氧化、氧化銅
相關次數：	點閱：98 下載：0
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本論文利用具有氧空洞的氧化釤添加氧化鈰（Samarium-Doped Ceria, 簡稱SDC）當載體，以含浸法將5wt%Cu擔載於擔體上，經500℃鍛燒製成觸媒。反應以氫氣作為載氣，通以定量的氧氣和CO，觀察其與載氣為Ar時的差異，及氫氣消耗的變化，發現在氫氣下CO的轉化率較低，認為氫氣的存在會於觸媒表面生成OH基，而抑制CO氧化反應的進行，至於氫氣的消耗情形，發現操作溫度在80∼120℃時，H2的消耗量不大，但CO的轉化率不高；而當溫度超過130℃時，雖然提高了CO的轉化率，卻會造成H2的大量消耗，而此溫度之取決，完全受限制於CO和H2對界面間氧原子的作用力，而TPRα波峰出現的溫度關係著反應起燃的溫度。在升溫和降溫測試中，認為遲滯現象的存在除了是穩定的界面活性位和熱點外，氧化銅群集形成亞穩態的表面活性位，也是造成遲滯現象的原因之一。另外，也藉由觀察在160℃下時，CO和H2競爭氧活性位的情形，發現與氫氣相較之下，CO對氧的反應力較強，故能使觸媒具有選擇性。在SDC擔體的製備方面，以水、乙醇、八醇三種不同的溶液製備擔體，使其造成不同的擔體表面積，而5wt%銅擔於較大表面積的擔體時，具有較多的界面活性位，故有較高的CO轉化率，然而，相對的使氫氣更易與氧發生反應。對於CuO/SDC觸媒的適用性，由實驗結果中評估，認為只要能提高此觸媒在低溫時的轉化率，即能使其成為具應用價值的材料。

第一章、     前言                                         1
第二章、     文獻回顧                                     3

1  燃料電池的發展                                   3

2  選擇氧化的研究                                   6

3  觸媒材料的選擇                                   7

4  提升活性的原理                                  10

5  導氧離子材料－SDC                               12

6  程溫還原                                        14

第三章、     實驗方法與步驟                              16

1  觸媒製備                                        16

1.1  藥品

1.2  製備方法

2  活性測試系統                                    21

2.1  儀器

2.2  活性測試步驟

2.3  數據處理

3  程溫還原測試                                    25

3.1  一氧化碳程溫還原

3.2  氫氣程溫還原

4  觸媒鑑定                                        26

4.1  X-光繞射（X-Ray Diffraction，XRD）

4.2  粒徑量測

4.3  氮氣物理吸附表面積

第四章、     實驗結果                                    29

1  CuO/SDC對CO選擇氧化的反應特性                   29

2  CuO/SDC活性衰退情形及反應後還原波峰             34

3  不同前處理對CuO/SDC觸媒的影響                   37

4  氧分壓及觸媒量對選擇氧化的影響                  39

5  不同表面積的SDC對CuO/SDC觸媒的影響              42

6  CO和H2競爭反應的情形                            45

7  基本金屬氧化物於SDC上之CO氧化活性               50

8  氧化鈷在不同製備下之活性比較                    53

第五章、     討論                                        55

1  觸媒活性座的變化情形                            56

2  Bulk銅的影響                                    60

3  擔體表面積的影響                                62

4  氧化鈷的活性                                    64

5  CuO/SDC觸媒對選擇氧化的適用性                   67

第六章、     結論                                        69

第七章、     建議及未來方向                              71

第八章、     參考文獻                                    72

附錄                                                 80

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