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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 劉雅瑄(Ya-Hsuan Liou) | |
dc.contributor.author | Yu-Thung Liaw | en |
dc.contributor.author | 廖宇同 | zh_TW |
dc.date.accessioned | 2021-06-17T01:09:36Z | - |
dc.date.available | 2021-01-21 | |
dc.date.copyright | 2020-01-21 | |
dc.date.issued | 2020 | |
dc.date.submitted | 2020-01-17 | |
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Synthesis, characterization and catalytic properties of CuO nanocrystals with various shapes. Nanotechnology, 17(15), 3939. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/66853 | - |
dc.description.abstract | 層狀雙氫氧化物(Layered double hydroxides, LDHs)一種陰離子型黏土,具有成本低廉、以及與金屬觸媒有協同作用已被視為有潛力的觸媒載體之一。本研究利用共沉澱、剝層以及含浸三種不同的製備方式合成了三種LDH觸媒系統分別以Cu-LDH、D-LDH以及Cu/LDH命名。最後以一氧化碳氧化實驗結果篩選出含浸法製備的材料為氧化表現最佳的材料。含浸法製備的材料在有氧條件下於200°C轉化了90%的一氧化碳。在X光繞射分析可以發現,含浸法製備的20 wt% Cu/LDH材料因同時具有LDH與CuO的結晶型態,在氧化效果上相比於其他兩種觸媒系統具有更好的表現。初步推測LDH與CuO的協同作用是主導氧化的主要因素。含浸法製備的20 wt% Cu/LDH材料在經過300°C和500°C的煅燒後,可以發現在有氧條件下的氧化效果上也有明顯的差異。20 wt% Cu/LDH300具有最佳的轉化效果,於80°C開始轉化一氧化碳,在150°C就達到最高90%的轉化。而20 wt% Cu/LDH500於100°C開始轉化一氧化碳,在175°C就達到最高72%的轉化。在in-situ FTIR的實驗中可以發現造成這個差異的原因是由於在經過300°C煅燒後的材料中的碳酸根與銅有著更強的鍵結(2500 cm-1處的吸收峰) 。2500cm-1處的吸收峰在無氧氣的氧化實驗條件下會隨著溫度升高逐漸減弱並消失,結合質譜儀無氧條件氧化實驗結果觀測到二氧化碳的生成推測碳酸根在一氧化碳的氧化中是一個提供氧的角色。另外,從質譜儀無氧條件氧化實驗結果、X光電子光譜以及X光繞射分析反應後的材料,可以發現在無氧條件下反應,材料中的氧化銅在150°C就完全被還原為0價的金屬銅。本研究結果發現層狀雙氫氧化物會參與一氧化碳氧化的反應中,並扮演著提供氧的角色,降低反應啟動溫度提升氧化效率。 | zh_TW |
dc.description.abstract | Layered double hydroxides(LDHs) is an anionic clay, one of the catalyst supporter that has been considered to have potential because of its low cost and synergistic effect with metal catalyst. In this research, 3 LDH catalyst were synthesized by co-precipitation, exfoliation and impregnation methods. The catalyst prepared by impregnation method has the best performance in oxidation of carbon monoxide. It converts 90% of carbon monoxide under O2 condition at 200°C. The synergistic effect between CuO and LDH was believed to be the main reason of better performance in oxidation of carbon monoxide.After calcination at 300°C and 500°C, it can be found that there is a significant difference in the carbon monoxide conversion performance under O2 condition. The catalyst calcined at 300°C has the best activity, CO started convert at 80°C and reach its maximum conversion of 90% at 150°C. However, the catalyst calcined at 500°C started convert CO at 100°C and reach its maximum conversion of 72% at 175°C. The in-situ FTIR experiment show that, reason for this difference is that the carbonate in the material after calcination at 300°C has stronger bonding with copper (absorption peak at 2500 cm-1). In the oxygen free experimental condition, the absorption peak at 2500 cm-1 decreased and disappeared as the temperature increased, combine the results of CO2 generation show by mass spectrometer, it shows that carbonate is a O supplier in this reaction. Copper oxide in catalyst is completely reduce to copper at 150°C proven by the results of XPS and XRD analysis of the catalyst after reaction. The result of this study found that LDH will participate in the oxidation of CO and play the role of providing oxygen, reducing the reaction starting temperature and increasing the oxidation efficiency. | en |
dc.description.provenance | Made available in DSpace on 2021-06-17T01:09:36Z (GMT). No. of bitstreams: 1 ntu-109-R06224115-1.pdf: 3825471 bytes, checksum: a008afb9b5835f98f712ada4e8740459 (MD5) Previous issue date: 2020 | en |
dc.description.tableofcontents | 中文摘要 I
Abstract IV 圖目錄 IX 表目錄 XII 第一章 緒論 1 1.1 研究緣起 1 1.2 研究目的 2 第二章 文獻回顧 3 2.1 一氧化碳氧化觸媒 3 2.1.1 鉑族金屬觸媒 3 2.1.2 金觸媒 6 2.1.3 銅與其他過渡金屬觸媒 10 2.2 影響銅觸媒一氧化碳催化氧化活性的變因 18 2.2.1 觸媒顆粒大小 18 2.2.2 觸媒製備方法 18 2.2.3 觸媒煅燒溫度的影響 18 2.2.4 氫氧基的影響 19 2.2.5 觸媒載體的影響 19 2.3 層狀雙氫氧化物(Layered double hydroxide,LDHs) 21 2.3.1 層狀雙氫氧化物背景介紹 21 2.3.2 層狀雙氫氧化物基本特性 21 2.3.3 層狀雙氫氧化物的製備方法 22 2.3.4 層狀雙氫氧化物的熱穩定性與記憶效應 25 2.3.5 層狀雙氫氧化物於各個研究領域中的應用 26 第三章 實驗設備及方法 29 3.1 實驗架構及內容 29 3.2 材料製備 31 3.2.1 共沉澱法製備含銅層狀雙氫氧化物Cu-LDH 31 3.2.2 製備含銅LDH奈米層片D-LDH 31 3.2.3 濕式含浸法負載銅於層狀雙氫氧化物載體 Cu/LDH 32 3.2.4 一氧化碳氧化實驗流程 33 3.3 特徵分析 34 3.3.1 X-光繞射光譜(X-ray Diffraction) 34 3.3.2 場發射掃描式電子顯微鏡(SEM) 34 3.3.3 比表面積分析儀(BET) 35 3.3.4 質譜儀(Mass spectrometry) 38 3.3.5 X光吸收光譜儀(X-ray absorption spectroscopy) 38 3.3.6 X-射線光電子能譜儀(X-ray photoelectron spectroscopy) 40 3.3.7 傅立葉轉換紅外光譜(Fourier-transform infrared spectroscopy) 40 第四章 結果與討論 41 4.1 三種製備方式合成含銅LDH之特性分析 42 4.1.1 晶相分析 42 4.1.2 比表面積分析 47 4.1.3 形貌分析 51 4.1.4 一氧化碳氧化實驗 53 4.1.5 含浸銅含量所造成的反應差異 54 4.1.6 煅燒溫度所造成的反應差異 55 4.1.7 熱重分析 56 4.2 不同煅燒溫度所造成的一氧化碳氧化效果差異 58 4.2.1 X-射線吸收光譜分析 58 4.2.2 X-射線光電子光譜分析 59 4.2.3 原位傅立葉轉換紅外光譜分析 61 4.2.4 無氧條件一氧化碳氧化實驗 67 4.2.5 有氧及無氧條件反應前後X光繞射分析 69 4.2.6 有氧及無氧條件反應前後X射線光電子光譜分析 72 4.3 機制探討 76 4.3.1 銅負載LDHs於無氧條件下之反應機制 76 4.3.2 銅負載LDHs於有氧條件下之反應機制 77 第五章 結論與建議 79 5.1 結論 79 5.2 建議 81 參考文獻 82 | |
dc.language.iso | zh-TW | |
dc.title | 氧化銅負載層狀雙氫氧化物於一氧化碳氧化之研究 | zh_TW |
dc.title | Layered double hydroxide supported CuO on carbon monoxide oxidation | en |
dc.type | Thesis | |
dc.date.schoolyear | 108-1 | |
dc.description.degree | 碩士 | |
dc.contributor.coadvisor | 林進榮(Chin-Jung Lin) | |
dc.contributor.oralexamcommittee | 胡景堯(Ching-Yao Hu),張瓊芬(Chiung-Fen Chang) | |
dc.subject.keyword | 層狀雙氫氧化物,協同作用,一氧化碳氧化, | zh_TW |
dc.subject.keyword | Layered double hydroxides,synergistic effects,carbon monoxide oxidation, | en |
dc.relation.page | 100 | |
dc.identifier.doi | 10.6342/NTU202000174 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2020-01-17 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 地質科學研究所 | zh_TW |
顯示於系所單位: | 地質科學系 |
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