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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 姜昌明 | zh_TW |
| dc.contributor.advisor | Chang-Ming Jiang | en |
| dc.contributor.author | 凃冠竹 | zh_TW |
| dc.contributor.author | Guan-Zhu Tu | en |
| dc.date.accessioned | 2025-08-21T16:47:49Z | - |
| dc.date.available | 2025-08-22 | - |
| dc.date.copyright | 2025-08-21 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2025-08-05 | - |
| dc.identifier.citation | (1) Agency, I. E. Global Energy Review 2023; Paris, 2023. https://www.iea.org/reports/world-energy-outlook-2023 (accessed 2025-06-09).
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/99203 | - |
| dc.description.abstract | 釩酸鉍（BiVO4）是一種具潛力應用於光電催化（photoelectrocatalytic, PEC）水分解與氧化反應的光陽極材料。然而，受限於真空製程的複雜性，其晶面依賴性催化行為尚未獲得充分研究。為克服此限制，本研究開發了一種結合金屬有機分解法（metal-organic decomposition, MOD）和快速熱退火（rapid thermal annealing, RTA）的溶液製程，用以合成BiVO4磊晶薄膜。此製程促進了奧斯特瓦爾德熟成（Ostwald ripening）並有效抑制了高溫下釩的損失。藉由優化熱處理條件，我們成功透過此方法在單晶YSZ和SrTiO3基板上生長出BiVO4 (001) 與 BiVO4 (010) 磊晶薄膜，並透過 X-ray 繞射與電子顯微鏡技術建立其磊晶成長機制。該溶液法製程克服真空法中常見的島狀生長問題，並獲得結構均勻、緻密且表面粗糙度低的薄膜。在光催化測試中，BiVO4 (010) 薄膜在羅丹明B降解中表現出相較於 (001) 晶面高約50%的反應效率，顯示其優異的晶面反應性。為進一步實現光陽極整合，本研究引入了氧化銦錫（indium tin oxide, ITO）作為導電背電極。儘管高溫退火有助於提高ITO的結晶性和導電性，但同時也使表面粗化，不利於後續BiVO4的生長。藉由在氬氣氛下進行後退火處理，可兼顧表面平整度並提升導電性。最終製備之 BiVO4 (001) /ITO/YSZ 光陽極在含有0.5 M Na2SO3的磷酸鹽緩衝液中展現出2.20 mA cm⁻2光電流密度，起始光電位約為 0.3 V (vs. RHE)。與對應多晶薄膜相比，具 (001) 晶向的 BiVO4 顯示出顯著提升的 PEC 效能，歸因於其增強的方向性電荷分離效率與表面復合抑制。阻抗分析亦顯示，特定晶向可有效促進界面電荷轉移。本研究展現了溶液法製備具生長取向氧化物磊晶薄膜的可行性，並有助於設計更高效的光電化學能量轉換裝置。 | zh_TW |
| dc.description.abstract | Bismuth vanadate (BiVO4) is a promising photoanode for photoelectrocatalytic (PEC) water splitting and oxidation, but its facet-dependent catalytic behavior remains underexplored due to reliance on complex vacuum-based fabrication. To address this, we developed a solution-based method combining metal–organic decomposition (MOD) and rapid thermal annealing (RTA) to grow epitaxial BiVO4 thin films. This process promotes Ostwald ripening and minimizes vanadium loss at elevated temperatures. Using this method, we successfully grew BiVO4(001) and (010) epitaxial films on single-crystal YSZ and SrTiO3 substrates, respectively. Through optimization of annealing conditions and structural analysis via XRD and electron microscopy, we established a model for solution-derived epitaxial growth, overcoming the island growth commonly observed in vacuum-based methods and yielding films with high structural uniformity, compactness, and low surface roughness. In photocatalytic testing, BiVO4(010) films exhibited approximately 50% higher activity than the (001) film in Rhodamine B degradation, indicating superior visible light absorption and surface reactivity. To realize photoanode integration, indium tin oxide (ITO) was introduced as a conductive back contact. Although high-temperature annealing enhanced ITO crystallinity and conductivity, it also deteriorated surface morphology, impeding epitaxial BiVO4 growth. A post-annealing step in an argon atmosphere was thus employed to improve conductivity while preserving surface flatness. The resulting BiVO4(001)/ITO/YSZ photoanodes delivered a photocurrent of 2.20 mA cm⁻2 and an onset potential of 0.3 V vs. RHE in phosphate buffer with 0.5 M Na2SO3 sacrificial hole scavenger. Compared to polycrystalline films, (001)-oriented BiVO4 showed enhanced PEC performance, attributed to enhanced directional charge separation and suppressed surface recombination. Impedance analysis further confirmed that specific crystallographic orientations enhance interfacial charge transfer. This study demonstrates the feasibility of using a solution-based approach to control the crystallographic orientation of oxide epitaxial thin films and contributes to the design of more efficient photoelectrochemical energy conversion devices. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2025-08-21T16:47:49Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2025-08-21T16:47:49Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 口試委員會審定書 i
Acknowledgements ii 中文摘要 iv Abstract vi Table of Contents viii List of Abbreviation xiii List of Figures xvii List of Tables xxxiii Chapter 1 Introduction 1 1.1 Solar Energy Conversion 1 1.1.1 Renewable Energy and Solar Utilization 1 1.1.2 Work Principles of Photoelectrocatalysis 2 1.2 Photoanode Design and Selection 6 1.2.1 Band Edge and Band Gap Requirement 6 1.2.2 Charge Separation and Carrier Transport 9 1.2.3 Light Absorption and Stability 11 1.2.4 Oxides-Based Photoanodes 12 1.2.5 Water Splitting Mechanism and Challenge 14 1.3 Bismuth Vanadate Photoanodes 16 1.3.1 Crystal Structure and Advantages 16 1.3.2 Intrinsic Limitations 21 1.3.3 Performance Improving Strategies 22 1.3.4 Anisotropic Properties 25 1.4 Epitaxial BiVO4 Thin Films 27 1.4.1 Facet-Dependent Transport and Catalytic Behavior of BiVO4 27 1.4.2 Epitaxial Films for Anisotropic Analysis 33 1.5 Epitaxial Synthesis Strategy 36 1.5.1 Criteria of Epitaxial Growth 36 1.5.2 Vacuum-Based Methods 39 1.5.3 Chemical Solution Epitaxy 45 1.5.4 Integration of RTA into the MOD Process 47 Chapter 2 Experimental Methods 51 2.1 Thin Film Deposition 51 2.1.1 Chemical Solution Deposition 51 2.1.2 Metal-Organic Decomposition 52 2.1.3 Principles of Spin Coating 53 2.1.4 Rapid Thermal Annealing 54 2.1.5 Sputter Deposition 57 2.2 Crystallographic and Compositional Analysis 60 2.2.1 X-ray Diffraction Analysis 60 2.2.2 Raman Spectroscopy 63 2.2.3 X-Ray Photoelectron Spectroscopy 66 2.2.4 X-ray Absorption Near Edge Structure 68 2.2.5 Inductively Coupled Plasma Mass Spectrometry 71 2.3 Morphological and Microstructural Characterization 73 2.3.1 Atomic Force Microscopy 73 2.3.2 Scanning Electron Microscopy 76 2.3.3 Energy Dispersive X-ray Spectroscopy 80 2.3.4 High-Resolution Transmission Electron Microscopy 82 2.4 Ultraviolet-Visible Spectroscopy 84 2.5 Four-Point Probe Measurement 86 2.6 Photoelectrochemical Characterization 89 2.6.1 Linear Sweep Voltammetry 92 2.6.2 Chronoamperometry 94 2.6.3 Electrochemical Impedance Spectroscopy 95 Chapter 3 Fabrication of Epitaxial BiVO4/YSZ and BiVO4/SrTiO3 Thin Films 101 3.1 Deposition of Epitaxial BiVO4 Films on YSZ(001) 101 3.1.1 BiVO4/YSZ Thin Film Fabrication Procedure 102 3.1.2 Influence of Annealing Method 104 3.1.3 Influence of Annealing Dwell Temperature 113 3.1.4 Influence of Annealing Heating Ramp Rate 116 3.1.5 Influence of Annealing Dwell Time with Different Film Thicknesses 119 3.1.6 Transformation Mechanism 128 3.2 In-Plane Epitaxial Relation of Optimized BiVO4/YSZ Thin Films 134 3.3 Doping Strategy and Characterization 137 3.4 Deposition of Epitaxial BiVO4 Films on SrTiO3(001) 145 3.4.1 BiVO4/STO Thin Film Fabrication Procedure 147 3.4.2 Characterization of BiVO4/SrTiO3 148 3.5 Applying Epitaxial BiVO4 Films for Photocatalysis 155 3.5.1 Analysis of optical properties 155 3.5.2 Photocatalytic Degradation of Rhodamine B 157 Chapter 4 Fabrication of Epitaxial ITO Films on YSZ(001) 162 4.1 Deposition Procedure of ITO/YSZ thin films 163 4.2 Effect of Synthesis Conditions on the ITO/YSZ Films 165 4.2.1 Two-Step Annealing Process 166 4.2.2 Influence of Precursor Composition 170 4.2.3 Optimization of Two-Step Annealing Process 174 4.2.4 Influence of Annealing Atmosphere 177 4.2.5 One-Step Annealing Process 179 4.2.6 Influence of Annealing Dwell Time 184 4.2.7 Influence of Annealing Temperature 187 4.3 Conductivity Analysis 192 4.3.1 Effect of annealing temperature on ITO conductivity 192 4.3.2 Effect of Post-Annealing 195 4.4 Optical Properties 198 Chapter 5 Epitaxial BiVO4/ITO/YSZ and Their Photoelectrochemical Performance 200 5.1 Deposition Procedure of BiVO4/ITO/YSZ Photoanode 200 5.1.1 BiVO4/ITO/YSZ Thin Film Fabrication Procedure 200 5.1.2 Preliminary Process Optimization for BiVO4/ITO/YSZ 203 5.1.3 Influence of BiVO4 One-Step Annealing Pyrolysis Temperature 207 5.1.4 Influence of Heat Treatment Atmosphere 213 5.1.5 Effect of ITO Thickness on BiVO4 Fabrication 219 5.1.6 Influence of BiVO4 Annealing Dwell Temperature 221 5.1.7 Influence of Annealing Dwell Time 225 5.1.8 Effect of ITO/YSZ Annealing Dwell Temperature 228 5.1.9 High-Resolution X-Ray Diffraction 230 5.2 Characterization of BiVO4/ITO/YSZ Photoanodes 231 5.2.1 Raman Spectroscopy 231 5.2.2 Pole Figure Analysis 233 5.2.3 High-Resolution Transmission Electron Microscopy 240 5.3 Photoelectrochemical Performance 244 5.3.1 Effect of Annealing Conditions on PEC Performance 244 5.3.2 PEC Characterization of Optimized BiVO4/ITO/YSZ Photoanodes 248 5.3.3 Electrochemical Impedance Analysis 256 Chapter 6 Conclusion 261 REFERENCE 263 | - |
| dc.language.iso | en | - |
| dc.subject | 磊晶釩酸鉍薄膜 | zh_TW |
| dc.subject | 光電催化水分解 | zh_TW |
| dc.subject | 氧化銦錫薄膜 | zh_TW |
| dc.subject | 快速熱退火 | zh_TW |
| dc.subject | 溶液法製程 | zh_TW |
| dc.subject | Solution-Based Deposition | en |
| dc.subject | Indium Tin Oxide Thin Films | en |
| dc.subject | Epitaxial Bismuth Vanadate Thin Films | en |
| dc.subject | Photoelectrochemical Water Splitting | en |
| dc.subject | Rapid Thermal Annealing | en |
| dc.title | 溶液法製備磊晶釩酸鉍薄膜: 合成、鑑定與催化性能研究 | zh_TW |
| dc.title | Solution-Derived Epitaxial BiVO4 Films for Phototelectrocatalytic Applications: Synthesis, Characterization, and Catalytic Performance | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 113-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 陳俊顯;廖尉斯;陳俊維 | zh_TW |
| dc.contributor.oralexamcommittee | Chun-Hsien Chen;Wei-Ssu Liao;Chun-Wei Chen | en |
| dc.subject.keyword | 光電催化水分解,磊晶釩酸鉍薄膜,溶液法製程,快速熱退火,氧化銦錫薄膜, | zh_TW |
| dc.subject.keyword | Photoelectrochemical Water Splitting,Epitaxial Bismuth Vanadate Thin Films,Solution-Based Deposition,Rapid Thermal Annealing,Indium Tin Oxide Thin Films, | en |
| dc.relation.page | 268 | - |
| dc.identifier.doi | 10.6342/NTU202503323 | - |
| dc.rights.note | 同意授權(限校園內公開) | - |
| dc.date.accepted | 2025-08-08 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 化學系 | - |
| dc.date.embargo-lift | 2026-08-01 | - |
| 顯示於系所單位： | 化學系 | |
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