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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 江建文 | zh_TW |
| dc.contributor.advisor | Kien Voon Kong | en |
| dc.contributor.author | 李明毅 | zh_TW |
| dc.contributor.author | Ming-Yi Lee | en |
| dc.date.accessioned | 2025-07-23T16:31:20Z | - |
| dc.date.available | 2025-07-24 | - |
| dc.date.copyright | 2025-07-23 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2025-07-18 | - |
| dc.identifier.citation | 1. Rosado, H. R. a. P., Fossil Fuels. Our World in Data 2017.
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/98030 | - |
| dc.description.abstract | 為滿足對具成本效益的水分解技術的迫切需求，亟需兼具高內在活性與長期穩定性的析氧反應(OER)電催化劑。本研究提出一種金屬有機框架（MOF）衍生的自犧牲策略以構建具有中空蛋黃-蛋殼結構的奈米棒，包括：(i)外層為CoNiFe層狀雙氫氧化物（LDH）、內核為CoFe-MIL的結構（CoFe-MIL@CoNiFe LDH YSNR），以及(ii)外層為NiFeSe2包覆Fe3O4的結構（Fe3O4@NiFeSe2 YSNR）。這種層級化中空結構可最大化電化學可接觸表面積、縮短離子擴散路徑，並穩定催化劑的活性相。在1.0 M KOH中，CoFe-MIL@CoNiFe LDH YSNR於過電位275 mV時可達10 mA cm⁻2的電流密度，Tafel斜率為94.8 mV dec⁻1；而Fe3O4@NiFeSe2 YSNR則於過電位260 mV時達相同電流，Tafel斜率為70.7 mV dec⁻1，均優於市售RuO2。恆電流測試顯示50小時內施加電位漂移小於4.5%，證明其優良的穩定性。電化學毒化實驗與去鐵對照實驗指出Ni/Co為主要活性位點，而Fe則透過協同電子效應提升催化表現。本研究證實，以MOF模板為導向的蛋黃-蛋殼合成策略為構建多金屬電催化劑的有效途徑，並為次世代高效析氧材料的設計提供了重要原則。 | zh_TW |
| dc.description.abstract | Meeting the urgent demand for cost effective water splitting technologies requires oxygen evolution electrocatalysts that couple high intrinsic activity with long term durability. Here we devise a metal-organic framework derived, self sacrificial strategy to construct yolk-shell nanorods comprising (i) a CoNiFe layered double hydroxide shell surrounding a CoFe MIL core (CoFe MIL@CoNiFe LDH YSNR) and (ii) a NiFeSe2 shell enclosing Fe3O4 (Fe3O4@NiFeSe2 YSNR). The hierarchical hollow architecture maximizes electrochemically accessible surface area, shortens ion diffusion pathways and stabilizes the active phase. In 1.0 M KOH, CoFe MIL@CoNiFe LDH YSNR attains a current density of 10 mA cm-2 at an overpotential of 275 mV with a Tafel slope of 94.8 mV dec-1, whereas Fe3O4@NiFeSe2 YSNR delivers the same current at 260 mV and 70.7 mV dec-1, surpassing commercial RuO2. Chronopotentiometry shows <4.5 % applied potential drift over 50 h, confirming great operational stability. Electrochemical poisoning and Fe free controls pinpoint Ni/Co sites as the primary OER centres, while Fe plays a synergistic electronic role. This work establishes MOF templated yolk-shell engineering as a powerful route to multi metallic electrocatalysts and provides design principles for next-generation oxygen-evolution materials. | en |
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| dc.description.provenance | Made available in DSpace on 2025-07-23T16:31:20Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | Acknowledgement i
摘要 ii Abstract iii Contents iv List of Figures vii List of Schemes xiii Chapter 1 Introduction 1 1.1 Hydrogen Energy 1 1.1.1 The Importance of Hydrogen Energy 2 1.1.2 The Approaches for Hydrogen Generation 3 1.1.3 Electrochemical Water splitting 4 1.2 Properties of Electrocatalysts 7 1.2.1 Non-Precious Transition-Metal Electrocatalysts 7 1.2.2 Metal-Organic Frameworks (MOFs) 9 1.2.3 Layer-Structured Oxide Materials 10 1.2.4 Hollow Nanostructures 13 1.3 Motivation 15 Chapter 2 Results and Discussion 16 2.1 Synthesis of MIL-88A@Nickel-Iron Layered Double Hydroxide Yolk-Shelled Nanorods 16 2.1.1 MIL-88A Nanorods 16 2.1.2 Polyvinylpyrrolidone Modified MIL-88A Nanorods 20 2.1.3 α-Ni(OH)2 21 2.1.4 MIL-88A@Nickel-Iron Layered Double Hydroxide Yolk-Shelled Nanorods 27 2.2 Synthesis of Cobalt-Iron MIL@Cobalt-Nickel-Iron Layered Double Hydroxide Yolk-Shelled Nanorods 44 2.3 Synthesis of Iron Oxide@Nickel-Iron Selenide Yolk-Shelled Nanorods 54 Chapter 3 Electrochemical Application–OER 63 3.1 Parameters of an Electrocatalyst for OER 63 3.1.1 Overpotential 63 3.1.2 Tafel Slope 65 3.1.3 Electrochemical Surface Area (ECSA) 66 3.1.4 Turnover Frequency (TOF) 68 3.2 OER Performance of the Electrocatalysts 70 3.2.1 OER Performance for MIL-88A, α-Ni(OH)2, MIL@NiFe-LDH YSNR 70 3.2.2 OER Performance for MIL@NiFe-LDH YSNR, CoFe-MIL@CoNiFe-LDH YSNR, Fe3O4@NiFeSe2 YSNR, and Commercial RuO2 74 3.2.3 Role of Iron in Enhancing OER Performance 80 3.2.4 Electrochemical Stability Test 81 3.2.5 Electrochemical Poisoning Studies for Active Site Identification 82 Chapter 4 Conclusion 83 Chapter 5 Experimental Section 85 5.1 General Information 85 5.2 Physical Measurements 87 5.3 Electrocatalytic OER Measurements 91 5.4 Preparation of Nanomaterials 94 Reference 99 Appendix 115 | - |
| dc.language.iso | en | - |
| dc.subject | 金屬硒化物 | zh_TW |
| dc.subject | 電催化 | zh_TW |
| dc.subject | 層狀雙氫氧化物 | zh_TW |
| dc.subject | 蛋黃-蛋殼結構 | zh_TW |
| dc.subject | 析氧反應 | zh_TW |
| dc.subject | Electrocatalysis | en |
| dc.subject | Oxygen Evolution Reaction | en |
| dc.subject | Yolk-shell structure | en |
| dc.subject | Layered Double Hydroxide | en |
| dc.subject | Metal selenide | en |
| dc.title | 具蛋黃-蛋殼結構之CoFe-MIL@CoNiFe-LDH與Fe3O4@NiFeSe2奈米棒作為高效析氧反應電催化劑之研究 | zh_TW |
| dc.title | Yolk-Shell Structured CoFe-MIL@CoNiFe-LDH and Fe3O4@NiFeSe2 Nanorods as High-Performance Electrocatalysts for the Oxygen Evolution Reaction | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 113-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 廖尉斯;陳重佑 | zh_TW |
| dc.contributor.oralexamcommittee | Wei-Ssu Liao;Chong-You Chen | en |
| dc.subject.keyword | 析氧反應,蛋黃-蛋殼結構,層狀雙氫氧化物,金屬硒化物,電催化, | zh_TW |
| dc.subject.keyword | Oxygen Evolution Reaction,Yolk-shell structure,Layered Double Hydroxide,Metal selenide,Electrocatalysis, | en |
| dc.relation.page | 117 | - |
| dc.identifier.doi | 10.6342/NTU202502031 | - |
| dc.rights.note | 同意授權(全球公開) | - |
| dc.date.accepted | 2025-07-18 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 化學系 | - |
| dc.date.embargo-lift | 2030-07-18 | - |
| 顯示於系所單位： | 化學系 | |
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