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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 牟中原 | |
dc.contributor.author | Meng-Liang Lin | en |
dc.contributor.author | 林孟良 | zh_TW |
dc.date.accessioned | 2021-06-08T06:00:58Z | - |
dc.date.copyright | 2007-07-31 | |
dc.date.issued | 2007 | |
dc.date.submitted | 2007-07-28 | |
dc.identifier.citation | References
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/25045 | - |
dc.description.abstract | 本研究的目標在於設計一高活性之直接甲醇燃料電池陽極觸媒,並探討催化活性與觸媒結構的關係。除了在具有最佳的甲醇電化學氧化反應性之鉑金屬觸媒中添加第二金屬觸媒—釕,以解決中間產物一氧化碳對鉑觸媒的毒化作用之外,亦將此鉑基合金觸媒擔載於具高表面積及特殊三度空間孔道排列的中孔碳載體上,大幅增加合金觸媒的分散度及活性表面積,更重要的是藉由降低甲醇氧化之反應物及產物的質傳效應,提高觸媒顆粒的利用率及催化性能。
以本實驗室發展之大面積垂直孔道排列的中孔洞氧化矽分子篩SBA-15(⊥)材料作為模版,以sucrose作為碳源,合成具高表面積(~1,100 m2/g)、高熱穩定性和孔道直徑4奈米、孔道長度80~150奈米的新穎薄膜形態中孔碳材。利用此孔洞結構碳材作為觸媒載體,以化學還原法於其表面負載鉑釕合金觸媒,並以化學半電池裝置測試甲醇電化學氧化反應之催化活性。 此外,利用臭氧在液相中進行中孔碳材表面修飾。我們發現,經修飾之碳材表面足以影響擔載過程中合金觸媒的成核作用及分散度,進而導致鉑釕合金程度的差異。實驗結果顯示,合金奈米顆粒表層成分為70% 鉑和30% 釕之化學組成具有最佳的甲醇氧化反應性。本論文結合X光光電子能譜及X光吸收光譜之分析結果,提出一鉑釕雙金屬合金顆粒結構模型,並建立了觸媒表面原子組成與甲醇電化學氧化之動力學機制的關連性。 最後,我們於雙金屬觸媒中加入非金屬元素—磷,以縮小觸媒顆粒的尺寸。實驗結果顯示,觸媒顆粒大小為3奈米的三元合金觸媒具有最佳甲醇電化學活性及催化穩定性。 | zh_TW |
dc.description.abstract | Well-ordered mesoporous carbon thin film with short nanochannels is synthesized and applied to direct methanol fuel cell as the anode PtRu alloy catalyst support. The enhancement of the electrooxidation of methanol is attributed to the increase of active sites and the catalyst utilization efficiency. The mass-transport effect on the diffusion of fuel molecules to the active metal sites is effectively minimized by the unique thin film morphology of the mesoporous carbon. Furthermore, a facile and environmental friendly method for surface modification of mesoporous carbon by ozone treatment is achieved. Presumably, the modification process may affect the nucleation and dispersion of the PtRu nanoparticles which then to deposit onto carbon surface. The bimetallic PtRu alloy with 70% Pt and 30% Ru surface atom ensemble is discovered to be the most favorable composition toward the kinetics of methanol electrooxidation. We also propose a structure model of carbon-supported PtRu nanoparticles through the results of X-ray photoelectron spectroscopy and X-ray absorption spectroscopy analyses. In addition, a non-metallic element, phosphorus, is added into PtRu alloy to reduce the particle size. The carbon-supported PtRuP nanocatalyst with particle size ~3.0 nm is found to possess both better reactivity and stability. | en |
dc.description.provenance | Made available in DSpace on 2021-06-08T06:00:58Z (GMT). No. of bitstreams: 1 ntu-96-F91223021-1.pdf: 8926870 bytes, checksum: c2b9dfd07faa9d9cbb3557107c5e244c (MD5) Previous issue date: 2007 | en |
dc.description.tableofcontents | Table of Contents
摘要 I Abstract II Table of Contents III List of Figures V List of Tables XI List of Schemes XIII Chapter 1 Introduction 1 1.1 Motivation and Goal 1 1.2 Direct Methanol Fuel Cell (DMFC) 3 1.3 Anode Catalysts of DMFC 6 1.4 Nanostructured Silica Materials 9 1.5 Nanostructured Carbon Materials 13 1.6 Dissertation Organization 16 Chapter 2 Well-Ordered Mesoporous Carbon Thin Film as a Nanocatalysts Support for DMFC Application 17 2.1 Introduction 17 2.2 Experiments 20 2.2.1 Synthesis of Mesoporous Silica Template SBA-15(⊥) 20 2.2.2 Synthesis of Mesoporous Thin Film Carbon (TFC) 20 2.2.3 Mesoporous Carbon of Other Categories Synthesized 21 2.2.4 Preparation of Mesoporous Thin Film Carbon Supported Bimetallic Nanocatalysts 24 2.2.5 Characterization Methods 24 2.3 Results and Discussion 29 2.3.1 Physical Chemical Characterization 30 2.3.2 Electrochemical Property 56 2.3.3 Nanocatalysts with Different Loading Extent 66 2.4 Conclusion 69 Chapter 3 Remarkable Supporting Effect via Surface Treatment of Mesoporous Carbon by Ozone 71 3.1 Introduction 71 3.2 Experiments 74 3.2.1 Ozone Treatment on Mesoporous Carbon 74 3.2.2 Strong Acid Treatment on Mesoporous Carbon 74 3.2.3 Preparation of Surface-Modified Mesoporous Carbon Supported Bimetallic Nanocatalysts 75 3.2.4 Characterization Methods 75 3.3 Results and Discussion 77 3.3.1 Physical Chemical Characterization 78 3.3.2 Electrochemical Property 87 3.3.3 X-ray Photoelectron Spectroscopy 99 3.3.4 X-ray Absorption Spectroscopy Technique 110 3.3.5 Bimetallic Nanocatalysts with Various Elemental Ratios 122 3.3.6 Toward a Mechanism for Methanol Electrooxidation and CO Oxidation 131 3.3.7 Proposed Structure Model of Mesoporous Carbon Supported PtRu Nanocatalysts and Ozone Effect 133 3.4 Conclusion 137 Chapter 4 The Third Element Combined PtRu Bimetallic Nanocatalysts and Size Effect 139 4.1 Introduction 139 4.2 Experiments 142 4.2.1 Preparation of Mesoporous Carbon Supported Ternary Pt-Ru-P Nanocatalysts 142 4.2.2 Characterizations 142 4.3 Results and Discussion 143 4.3.1 Structure Characterization of the Nanocatalysts 143 4.3.2 Electrochemical Property 146 4.3.3 Size Effect on the Ternary Nanocatalysts 150 4.4 Summary 158 Chapter 5 Conclusion and Outlook 159 Reference 165 Appendix 173 | |
dc.language.iso | en | |
dc.title | 中孔洞碳材應用於直接甲醇燃料電池陽極觸媒 | zh_TW |
dc.title | Ordered Mesoporous Carbon Applied Direct Methanol Fuel Cell Anode Catalysts | en |
dc.type | Thesis | |
dc.date.schoolyear | 95-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 陳貴賢,劉尚斌,盧敏彥,林昇佃 | |
dc.subject.keyword | 中孔洞碳材,直接甲醇燃料電池,鉑釕合金觸媒,表面修飾,臭氧,X光光電子能譜,X光吸收光譜, | zh_TW |
dc.subject.keyword | Ordered Mesoporous Carbon,Direct Methanol Fuel Cell,PtRu Alloy Catalyst,Surface Treatment,Ozone,X-ray Photoelectron Spectroscopy,X-ray Absorption Spectroscopy, | en |
dc.relation.page | 177 | |
dc.rights.note | 未授權 | |
dc.date.accepted | 2007-07-30 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
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