直接生長過渡金屬氧化物於超級電容器電極之應用研究

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姓名

楊尚仁(Sang-Ren Yang) 查詢紙本館藏

畢業系所

材料科學與工程研究所

論文名稱

直接生長過渡金屬氧化物於超級電容器電極之應用研究
(Direct Growth of Transition Metal Oxides (TMOs) on Electrodes for Supercapacitor Applications)

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摘要(中)

石油的枯竭、可再生能源的發展、電動車以及消費性電子裝備的廣泛應用，導致對各式能源儲存的需求不斷增加。電化學在各種能源儲存技術中扮演著關鍵角色，因此開發高性能的電極材料更顯重要。過渡金屬氧化物(transition metal oxides, TMOs)，因可提供多價態和多活性位點，在電極中可做為關鍵的活性物質，但卻也有低導電性與活化能力被電極加工方式降低的問題。因此在本研究探討了直接生長TMOs用於超級電容器電極，主要關注兩個主題：可撓式電極和高熵氧化物(high entropy oxide, HEO)電極。
在可撓式電極研究中，我們使用了電紡絲的方法製作出具有銀顆粒的奈米碳纖維 (CNF/Ag) 基材，並以原位氧化還原(in-situ redox)方式於基材上直接生長二氧化錳(MnO2)，最終形成MnO2-CNF/Ag的電極，這樣的架構提高了整體的導電性和電化學性能與電極的可撓性，其在1 A/g的電流密度下具有184 F/g，為CNF電極的17倍，並有16.3 Wh/kg的能量密度和400 W/kg的功率密度；在1,200次循環充、放電測試下仍可保持95 %的電容維持率，並在0-5cm曲率半徑下達到87 %的電容維持率。
在HEO電極的研究中，我們使用含鈷、鉻、鐵、錳、鎳的TMOs作為活性材料，以脈衝雷射掃描方式直接生長HEO在鎳基板上。高熵材料獨特的組合特性導致了優異的性能，該電極在1 A/g電流密度下實現了870 F/g的電容值，以及22.3 Wh/kg的能量密度和212 W/kg的功率密度。並且在1,000次充、放電循環後，仍可保持82 %的電容維持率。
這些結果證明了直接生長過渡金屬氧化物在超級電容器電極的可行性，並同時可提供良好的電化學性能。

摘要(英)

The depletion of petroleum, the rise of renewable energy, and the widespread use of electric vehicles and consumer electronics have increased the demand for energy storage. Electrochemistry is crucial in energy storage technologies, making the development of high-performance electrode materials vital. Transition metal oxides (TMOs) offer multiple valence states and active sites but suffer from low conductivity and reduced activation due to electrode fabricate processing. In this thesis explores the direct growth of TMOs for supercapacitor electrodes, focusing on flexible and high-entropy oxide (HEO) electrodes.
For flexible electrodes, we used electrospinning to fabricate a nanocarbon fiber substrate with Ag (CNF/Ag). MnO2 was directly grown on CNF/Ag via in-situ redox reaction, forming MnO₂-CNF/Ag electrode. This structure improved conductivity, flexibility and electrochemical performance. The electrode achieved 184 F/g at 1 A/g, which is 17 times higher than CNF electrodes, with an energy density of 16.3 Wh/kg and a power density of 400 W/kg. The capacitance retention exhibited 87 % across various curvatures (r: 0-5cm), and also shown 95 % capacitance retention after 1,200 charge-discharge cycles.
In the study of HEO electrodes, we employed high entropy (Co, Cr, Fe, Mn, Ni) oxide as the active material, directly grown on Ni substrates. The unique properties of HEO resulted in outstanding performance. The HEO electrode achieved a specific capacitance of 870 F/g at 1 A/g, along with an energy density of 22.3 Wh/kg and a power density of 212 W/kg. The capacitance retention maintained 82 % after 1,000 cycles of charge-discharge.
These results demonstrate the feasibility of directly growing TMOs on electrodes and providing excellent electrochemical performance in supercapacitor.

關鍵字(中)

★ 二氧化錳
★ 奈米碳纖
★ 可撓式電極
★ 高熵金屬氧化物
★ 超級電容

關鍵字(英)

★ Manganese Dioxide
★ Carbon Nanofiber
★ Flexible Electrode
★ High-entropy (Co, Cr, Fe, Mn, Ni) oxides
★ Supercapacitor

論文目次

摘要 I
Abstract II
致謝 III
Table of contents IV
List of figures VII
List of tables XIV
Chapter 1 Introduction 1
1.1 Preface 1
1.2 Supercapacitor 7
1.2.1 Electrical double-layer capacitors 8
1.2.2 Pseudocapacitors 10
1.2.3 Hybrid-capacitors 13
1.2.4 Electrode for supercapacitor 14
1.2.5 Material for electrode 17
1.2.5.1 Carbon-based materials 17
1.2.5.2 Transition metal oxides 23
1.2.5.1 Binder 31
1.3 Improvement directions of electrode 32
1.4 Flexible electrode 34
1.4.1 Carbon-based flexible electrodes 35
1.4.2 CNF network electrodes 37
1.4.2.1 Electrospinning 37
1.4.2.2 Stabilization and carbonization 38
1.4.3 MnO2-CNF electrode 40
1.4.4 Improvement of MnO2-CNF electrode 44
1.4.4.1 Addition of conductive materials into MnO2 44
1.4.4.2 Addition of conductive materials into CNF 47
1.5 High entropy oxides electrode 50
1.5.1 Characteristics of high entropy oxides 51
1.5.2 Fabrication of high entropy oxides 53
1.5.3 Rapid methods 54
1.5.4 Applications in electrode 57
1.6 Motivation 60
Chapter 2 Experimental 63
2.1 Flexible electrode 63
2.1.1 CNF/Ag electrode 63
2.1.2 MnO2-CNF/Ag electrode 64
2.2 HEO electrode 65
2.2.1 Ni substrate 65
2.2.2 HEO/NP electrode 65
2.3 Characterization of the materials 67
2.4 Electrochemical performance 67
Chapter 3 Results and discussion 69
3.1 Flexible electrode 69
3.1.1 Direct growth of MnO2 on CNF/Ag 69
3.1.2 Electrochemical performance 74
3.1.3 Bending test 86
3.2 HEO/NP electrode 88
3.2.1 Direct growth of high-entropy (Co,Cr,Fe,Mn,Ni) oxides on Ni-pellet 88
3.2.2 Electrochemical performance 97
Chapter 4 Conclusions 106
Chapter 5 Future work and outlook 108
References 110

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指導教授

李勝偉(Sheng-Wei Lee)

審核日期

2024-7-18

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