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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 | 馮竣麟 | zh_TW |
| dc.contributor.author | Jun-Lin Fong | en |
| dc.date.accessioned | 2025-08-22T16:05:10Z | - |
| dc.date.available | 2025-08-23 | - |
| dc.date.copyright | 2025-08-22 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2025-08-13 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/99299 | - |
| dc.description.abstract | 單斜白鎢礦結構BiVO4 (ms-BiVO4) 具有間接能隙 (~2.4 eV) 的特性、適合的能帶位置，以及在廣泛工作條件下穩定的電化學性能，是一種很有前景的半導體光陽極，適用於高效光電化學(photoelectrochemical, PEC) 水分解。儘管具有優越的特性，ms-BiVO4 仍受到極化子躍遷導致的低電子遷移率，以及由於表面復合和光降解而導致的異質半導體-電解質界面 (semiconductor-electrolyte interface) 的電荷轉移動力學降低的影響。通過簡便的溶膠-凝膠製備方法，我們合成了沉積在FTO 基板上的多晶ms-BiVO4 光陽極，重點分析了光陽極界面上普遍存在的本徵表面缺陷態的作用。此外，採用基於PEC 的小擾動探測技術，通過分析不同濃度電洞清除劑的影響和使用不同電解質的效果，來解析各種實驗條件下不同的載流子動力學。因此，我們觀察到ms-BiVO4光陽極在陽極掃描過程中逐漸表現出多種主導現象，包括體相擴散/復合、表面陷阱/去陷阱和費米能階釘扎 (Fermi-level pinning)，每種現象都與其使用小擾動技術得到的獨特光譜特徵和趨勢相關。總結而言，我們定性地假設ms-BiVO4光陽極存在兩種不同的本徵表面態，這些表面態深刻影響界面能量學以及整體析氧反應(OER) 過程。 | zh_TW |
| dc.description.abstract | Monoclinic scheelite BiVO4 (ms-BiVO4), with a mainly indirect bandgap (~2.4 eV) character, suitable band position, and stable electrochemical performance within a wide range of working conditions, serve as a promising semiconductor photoanode for efficient photoelectrochemical (PEC) water splitting. Despite its superior features, ms-BiVO4 suffers from low electron mobility due to polaron hopping and reduced charge transfer kinetics at the heterogeneous semiconductor-electrolyte interface (SEI) due to surface recombination and photodegradation. Through facile sol-gel based fabrication method, we synthesis polycrystalline ms-BiVO4 photoanode deposited on FTO substrate, where we focus on analyzing the role of intrinsic surface defect states (i-SS) commonly exist on the photoanode interface. Furthermore, PEC-based small perturbation probing techniques were employed to deconvolute distinct carrier dynamics along various experimental conditions, through analyzing the impact of different concentration of hole scavenger and the usage of different electrolyte. Consequently, we observed that ms-BiVO4 photoanode gradually exhibit multiple dominating phenomenon during anodic scanning, which includes bulk diffusion/recombination, surface trapping/de-trapping and Fermi-level pinning (FLP), each associated with its unique spectral features and trends using small perturbation techniques. In conclusion, we qualitatively assumed that ms-BiVO4 photoanodes exhibit two distinctive intrinsic SS, which influence the interfacial energetics and thus the overall OER process profoundly. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2025-08-22T16:05:10Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2025-08-22T16:05:10Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 口試委員會審定書 i
Acknowledgement ii 中文摘要 iii Abstract iv Thesis Contents v List of Figures viii List of Tables xx Chapter 1 Introduction 1 1.1 Photoelectrochemical (PEC) Water Splitting 1 1.2 Bismuth Vanadate Photoanode 3 1.3 Fundamental Understanding of Photoelectrodes 5 1.3.1 Energy Band-Diagrams for Photoelectrodes 6 1.3.2 Intrinsic, Extrinsic Surface-states and Fermi-level Pinning 14 1.3.3 Electric Double Layer and Gouy-Chapman-Stern (GCS) Theory 23 1.3.4 Gärtner–Butler and Photocurrent Density Equation 29 1.4 Introduction of Small Perturbation Techniques 31 1.5 Basic Principles of Electrochemical Impedance Spectroscopy (EIS) 36 1.5.1 Transfer Functions and Complex Plane Plots 38 1.5.2 Equivalent Circuit Modeling in EIS Analysis 41 1.5.3 Randles Circuit and Infinite-Diffusion Warburg Impedance 44 1.5.4 Constant-Phase Dispersive Elements (CPE) 49 1.5.5 Finite-Diffusion Warburg Transmission-Line Model 52 1.5.6 Porous-Structured Transmission Line Model 56 1.5.7 Gerischer-Type Transmission Line Model 62 1.5.8 Surface Trapping/De-trapping for Semiconductors 65 1.6 Mott-Schottky Analysis for Semiconducting Photoanodes 70 1.7 Basic Principles of Intensity-Modulated Photocurrent Spectroscopy (IMPS) 74 1.7.1 Surface Trapping/De-trapping Representation in IMPS 77 1.7.2 Bulk Carrier Dynamics Representation in IMPS 79 Chapter 2 Experimental and Analytical Method 84 2.1 X-Ray Diffraction (XRD) 84 2.2 Ultraviolet and Visible Spectroscopy (UV-Vis) 85 2.3 Raman Spectroscopy 87 2.4 Scanning Electron Microscope (SEM) 88 2.5 X-Ray Photoelectron Spectroscopy (XPS) 89 2.6 Linear-Scan Voltammetry (LSV) 90 2.7 Cyclic Voltammetry (CV) 92 Chapter 3 Experimental Results and Discussions 95 3.1 Fabrication of BiVO4 Photoanode 96 3.2 Structural and Optical Characterization 97 3.2.1 XRD Analysis for BiVO4 Photoanode 97 3.2.2 UV-Vis and Raman Spectroscopy for BiVO4 Photoanode 98 3.2.3 SEM for BiVO4 Photoanode 100 3.2.4 XPS Analysis for BiVO4 Photoanode 101 3.3 Setup for Basic Photoelectrochemical Measurements 105 3.3.1 Linear-Sweep Voltammetry for BiVO4 Photoanode 108 3.3.2 Cyclic Voltammetry for BiVO4 Photoanode 109 3.4 Prerequisites for EIS and IMPS Analysis 111 Chapter 4 Impact of Hole Scavenger Concentration 115 4.1 EIS Nyquist Plot Analysis – Without Adding Hole Scavenger 115 4.2 EIS Bode Plot Analysis – Without Adding Hole Scavenger 118 4.3 EIS Nyquist Plot Analysis – Addition of Hole Scavenger 124 4.4 EIS Bode Plot Analysis – Addition of Hole Scavenger 128 4.5 Mott-Schottky Analysis for Hole Scavenger Experiment 134 4.6 EIS Circuit Fitting for Hole Scavenger Experiment 142 4.7 IMPS Analysis for Hole Scavenger Experiment 148 Chapter 5 Impact of Different Electrolyte Medium 157 5.1 EIS Nyquist Plot Analysis – Recap on Na2SO4 Electrolyte 157 5.2 EIS Bode Plot Analysis – Recap on Na2SO4 Electrolyte 159 5.3 EIS Analysis – Comparison Between Different Electrolyte 164 5.4 Mott-Schottky Analysis for Different Electrolyte Experiment 169 5.5 EIS Circuit Fitting for Different Electrolyte Experiment 173 5.6 IMPS Analysis for Different Electrolyte Experiment 180 Chapter 6 Conclusion and Outlook 186 References 188 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 光電催化 | zh_TW |
| dc.subject | 釩酸鉍光陽極 | zh_TW |
| dc.subject | 析氧反應 | zh_TW |
| dc.subject | 表面態 | zh_TW |
| dc.subject | Surface state | en |
| dc.subject | Oxygen evolution reaction | en |
| dc.subject | Bismuth vanadate photoanode | en |
| dc.subject | Photoelectrocatalysis | en |
| dc.title | 利用小訊號微擾技術解析釩酸鉍光陽極在光電催化水分解中的表面電荷載子動力學 | zh_TW |
| dc.title | Demonstration of Small Perturbation Techniques on Resolving Interfacial Carrier Dynamics in BiVO4 Photoanodes During PEC Water Splitting | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 113-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 周必泰;陳俊顯;陳嘉晉 | zh_TW |
| dc.contributor.oralexamcommittee | Pi-Tai Chou;Chun-Hsien Chen;Chia-Chin Chen | en |
| dc.subject.keyword | 光電催化,釩酸鉍光陽極,析氧反應,表面態, | zh_TW |
| dc.subject.keyword | Photoelectrocatalysis,Bismuth vanadate photoanode,Oxygen evolution reaction,Surface state, | en |
| dc.relation.page | 197 | - |
| dc.identifier.doi | 10.6342/NTU202504151 | - |
| dc.rights.note | 同意授權(限校園內公開) | - |
| dc.date.accepted | 2025-08-15 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 化學系 | - |
| dc.date.embargo-lift | 2026-06-01 | - |
| 顯示於系所單位： | 化學系 | |
文件中的檔案：
| 檔案 | 大小 | 格式 | |
|---|---|---|---|
| ntu-113-2.pdf 未授權公開取用 | 15.22 MB | Adobe PDF | 檢視/開啟 |
系統中的文件，除了特別指名其著作權條款之外，均受到著作權保護，並且保留所有的權利。