以離子交換法製備矽-鋁二元氧化物擔體鎳觸媒之研究

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姓名

楊家明(Chia-Ming Yang) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

以離子交換法製備矽-鋁二元氧化物擔體鎳觸媒之研究
(Preparation of RHA-Al2O3 Binary Oxide Supported Nickel Catalyst by Ion Exchange)

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摘要(中)

本研究以稻殼灰分為主原料，利用離子交換法製備矽-鋁二元氧化物擔體鎳觸媒，並於一大氣壓、573K ~ 923K下進行二氧化碳甲烷化反應活性測試，結果顯示矽-鋁二元氧化物擔體鎳觸媒於高溫下的熱穩定性能使甲烷化反應有高甲烷選擇率。
於觸媒製備方面，實驗結果發現：金屬載量愈低，則金屬分散度愈高；而適當的鍛燒程序，能夠控制觸媒表面金屬晶粒的大小及分佈，使其有較佳的催化活性。因此，欲使矽-鋁二元氧化物擔體鎳觸媒發揮最佳的催化效率，4.44 wt%的金屬載量、773K下4小時的鍛燒，由室溫升溫至773K的還原程序及923K下的甲烷化反應，將是最佳的製備及操作條件。且經由TPR及TPD技術的分析證實，以稻殼灰分製備而成的矽-鋁二元氧化物擔體﹙RHA-Al2O3﹚，其特殊的擔體表面性質有利於鎳金屬分散，乃是一種兼具高促進效果及經濟效益的甲烷化觸媒擔體。

摘要(英)

RHA-Al2O3 binary oxide supported nickel catalyst prepared by ion exchange was examined in methanation of CO2 at 573 ~ 923K and high selectivity for CH4 formation was found at high reaction temperature due to its thermal stability.
During the investigations of preparation conditions, effects of nickel loading, calcination temperature, calcination time, reaction time and reaction temperature on catalytic behavior were presented and discussed. The results indicate that the metal dispersion increases with decreasing of nickel loading; the CH4 selectivity depends on calcination conditions; the activity of nickel catalyst achieves a maximum value with a nickel loading of 4.44 wt% , calcined at 773K for 4h and reduced at 773K in CO2 hydrogenation at 973K.
Moreover, by using TPR and H2-TPD techniques, RHA-Al2O3 is good for the dispersion of nickel and is a preferable and economic support.

關鍵字(中)

★ 二氧化碳甲烷化
★ 鎳觸媒
★ 矽-鋁二元氧化物擔體
★ 稻殼灰分
★ 離子交換法

關鍵字(英)

★ CO2 methanation
★ nickel catalyst
★ RHA-Al2O3 binary oxide support
★ rice husk ash
★ ion exchange

論文目次

目錄
內容頁數
中文摘要………………………………………………………… Ⅰ
英文摘要………………………………………………………… Ⅱ
圖索引………………………………………………………… Ⅴ
表索引………………………………………………………… Ⅷ
第一章緒論…………………………………………………… 1
第二章文獻回顧……………………………………………… 6
2-1稻殼灰分的性質及製備程序………………………… 6
2-2矽-鋁二元氧化物擔體的性質……………………… 11
2-2-1氧化鋁擔體的性………………………… 11
2-2-2矽-鋁二元氧化物擔體的性質…………… 12
2-3以離子交換法製備擔體鎳觸媒……………………… 15
2-4擔體效應……………………………………………… 18
2-5二氧化碳甲烷化反應………………………………… 20
2-5-1二氧化碳甲烷化的反應機構…………… 21
2-5-2觸媒的選擇……………………………… 23
第三章實驗方法與裝置……………………………………… 25
3-1觸媒擔體的製備與分析……………………………… 25
3-1-1稻殼前處………………………………… 25
3-1-2觸媒擔體﹙RHA-Al2O3﹚的製備……… 31
3-1-3觸媒擔體﹙RHA-Al2O3﹚的分析……… 32
3-2Ni/RHA-Al2O3觸媒的製備與活性測試…………… 35
3-2-1鎳觸媒的製備…………………………… 35
3-2-2觸媒的活性測試─CO2甲烷化反應……… 36
3-3觸媒的鑑定分析……………………………………… 38
3-3-1ICP-AES分析、XRD分析及SEM分析……… 38
3-3-2程溫還原﹙TPR﹚………………………… 39
3-3-3氫氣的程溫脫附﹙H2-TPD﹚…………… 41
3-4實驗流程與操作變數………………………… 43
3-5數據的計算與實例……………………………… 44
3-6儀器及藥品……………………………………… 49
第四章理論分析……………………………………………… 52
4-1熱力學的分析………………………………………… 52
4-2動力學上的假設……………………………………… 54
第五章結果與討論…………………………………………… 55
5-1Ni/RHA-Al2O3製備條件的探討……………………… 55
5-1-1觸媒還原程序的探討…………………… 55
5-1-2金屬載量對觸媒活性的影響……………… 61
5-1-3鍛燒程序的探討………………………… 68
5-1-4反應時間的選擇………………………… 73
5-1-5反應溫度對於甲烷化反應的影響……… 79
5-2製備方法及擔體效應的反應活性比較…………… 81
第六章結論………………………………………………… 94
參考文獻……………………………………………………… 96
附錄實驗數據………………………………………………102

參考文獻

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指導教授

張奉文(Feg-Wen Chang)

審核日期

2000-7-6

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