博碩士論文 108223035 詳細資訊



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姓名 吳秉晏(Ping-Yen Wu)  查詢紙本館藏   畢業系所 化學學系
論文名稱 在銅奈米立方體上建構非均勻相雙金屬表 面以利費托合成之應用
(Fischer Tropsch Synthesis Reaction over Heterogeneous Bimetallic Surfaces on Single Cu Nanocubes)
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摘要(中) 自1970年代的能源危機之後，由於石油的短缺，使得全球開始重視替代性能源的生產，費托合成即是其中一個具有代表性的例子。費托合成可以透過催化劑與一氧化碳和氫氣的催化聚合反應，產生各種有價值的烴類產品。廣泛的研究集中在提高催化劑的活性與提升高價值化合物的選擇率。其中，由於合金材料的協同效應，包括電子效應和應變效應，使得由多元素組成的奈米催化劑效能優於單元素奈米催化劑。不僅如此，參雜少量的貴金屬促進劑可以進一步提升催化性能與產物選擇率。在此，我們設計了銅-銅鉑-銅鎳在結構上對應為核-框架-表面三金屬奈米催化劑的合成方法，不同於其他文獻中的三元合金催化劑，在本篇研究的催化劑中，其邊緣和頂點的材料為銅鉑合金，而表面的材料則為銅鎳合金。為了探討此催化劑在中每個成分與合金對費托反應的影響，我們合成了另一種銅-銅鉑-銅鈀三金屬催化劑做為比較，同時測試每個元素與合金在費托反應中的催化能力。在結果中，銅-銅鉑-銅鎳在所有材料中擁有最高的催化能力。除了費托合成的應用，由於此催化劑在單一奈米顆粒上擁有兩種不同的合金，它同時擁有在氣象中進行連續催化的能力。我們期望未來可利用其兩種不同材料的界面在於異質氣相催化反應中進行串聯催化。
摘要(英) Since the energy crisis in the 1970s, the world began to notice the importance of alternative energy sources due to the oil shortage. Fischer-Tropsch synthesis (FTS) reaction is one of the representative examples. FTS reaction can produce a variety of valuable hydrocarbon products through carbon monoxide and hydrogen catalyzed by catalysts. Extensive researches were focused on significantly increasing the selectivity of specific high economic value compounds and improving the activity of catalysts. In particular, multimetallic catalysts have better catalytic performance due to the synergy of electronic and strain effects. Additionally, introduce a small amount of promoter can further enhance the activity and product selectivity. In this research, we employed the synthesis of trimetallic Cu-CuPt-CuNi core-frame-face trimetallic nanocrystals. Different to typical alloy, this trimetallic nanostructure possesses CuPt alloy on edge and CuNi alloy on face. In order to investigate the effect of each element and alloy in FTS reaction. We synthesized another trimetallic nanocrystals Cu-CuPt-CuPd to compare and test the catalytic performance of each element and alloy. In the results, Cu-CuPt-CuNi shows the highest catalytic ability and conversion among the catalysts. In addition to the application of FTS reaction, owing to the two different alloys on the surface, Cu-CuPt-CuNi also has the potential for tandem catalysis. We expect this nanocrystal can be applied for heterogeneous gas phase tandem catalysis in near future.
關鍵字(中) ★ 銅鉑鎳
★ 銅鉑鈀
★ 核殼結構
★ 費托合成		 關鍵字(英) ★ CuPtNi
★ CuPtPd
★ core-shell
★ Fischer Tropsch Synthesis Reaction
論文目次 摘 要....................................i
ABSTRACT......................................ii
誌 謝.........................................iii
Table of Contents.............................iv
List of Figures...............................vii
List of Tables................................x
Chapter I Overview............................1
1-1 Research Background.......................1
1-2 Research Motivation.......................2
Chapter II Introduction.......................4
2-1 Fischer-Tropsch Synthesis.................4
2-1-1 Mechanism of Fischer-Tropsch synthesis (FTS) reaction......................................4
2-1-2 Active Materials........................5
2-1-3 Promoters...............................6
2-1-4 Bimetallic catalysts....................6
2-2 Nanomaterial..............................8
2-2-1 Nanocrystal.............................8
2-2-2 Shape-Controlled Synthetic Approach.....8
2-3 Tandem Catalysis..........................8
2-3-1 Concept of Tandem Catalysis of Nanocrystal Bilayers......................................8
2.3.2 Tandem Catalysis for CO2 Hydrogenation to C2-C4 Hydrocarbons..................................10
Chapter III Experimental section..............13
3-1 Chemicals.................................13
3-2 Procedure of Synthesis Catalyst...........13
3-2-1 Synthesis of Cu Nanocubes...............13
3-2-2 Synthesis of Rhombic Dodecahedral Cu-CuPt Core-Frame Nanocrystals..................................14
3-2-3 Synthesis of Cu-CuNi Core-Shell Nanocubes.....................................14
3-2-4 Synthesis of Rhombic Dodecahedral Cu-CuPt-CuPd Core-Frame-Face Nanocrystals.......................15
3-2-5 Synthesis of Rhombic Dodecahedral Cu-CuPt-CuPd Core-Frame-Face Nanocrystals.......................16
3-2-6 Synthesis of Rhombic Dodecahedral Cu-CuPt-CuNi Core-Frame-Face Nanocrystals.......................16
3-3 Procedure of Catalysis....................17
3-3-1 Fischer-Tropsch Process.................17
3-3-2 Heterogeneous Catalysis System..........17
3-4 Characterization..........................19
Chapter IV Results and discussion.............21
4-1 Structural Analysis of Cu-CuPt-CuNi Core-Frame-Face Trimetallic Nanocrystal.......................21
4-2 Structural Analysis of Cu-CuPt-CuPd Core-Frame-Face Trimetallic Nanocrystal.......................28
4-3 Catalytic Performance of Trimetallic and Comparisons toward Fischer-Tropsch Synthesis Reaction......................................35
Conclusions...................................45
Bibliography..................................46
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指導教授 謝發坤 郭俊宏(Fa-Kuen Shieh Chun-Hong Kuo) 審核日期 2021-7-26
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