請用此 Handle URI 來引用此文件:
http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/50947
完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 劉如熹 | |
dc.contributor.author | Chih-Jung Chen | en |
dc.contributor.author | 陳致融 | zh_TW |
dc.date.accessioned | 2021-06-15T13:08:19Z | - |
dc.date.available | 2021-10-05 | |
dc.date.copyright | 2016-10-05 | |
dc.date.issued | 2016 | |
dc.date.submitted | 2016-06-29 | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/50947 | - |
dc.description.abstract | 近期全球能源消耗速率每年約為15 TW,發展再生能源來取代石化燃料與核能為刻不容緩之研究,於1972年,Honda與Fujishima首度嘗試將太陽能轉變為化學能,並提出光催化水分解(solar water splitting)之概念,當使用水分解產生之氫氣時,環境友善之水蒸氣為其唯一產物,故光催化水分解為一理想解決全球能源危機之方式。於眾多不同之半導體中,矽材料(silicon; Si)因其較小之能隙與較負之導帶邊界,因此矽光陰材料可幾乎吸收全太陽光可見光光譜,並進行光催化產氫反應,而被視為極佳之光催化水分解陰極電極,然矽光陰極材料因光激發載子動能不足,使其光電化學表現不佳,此外當其接觸水溶液電解液時,於表面易生成絕緣之氧化層造成光催化活性衰退或去活性。於此論文中,三大主要策略被發展改善矽光陰極材料之效率與穩定性,表面電漿共振(surface plasmon resonance)金屬粒子與共催化劑(co-catalyst)材料用於提升矽光陰極材料之表現,此外鈍化層(passivation layer)則做為保護層提高其穩定度。 | zh_TW |
dc.description.abstract | The current global energy consumption rate is approximately 15 TW per year. Developing a renewable energy resource as a substitute for fossil fuels and nuclear power is a research topic that needs attention. In 1972, Honda and Fujishima first demonstrated the conversion of solar energy into chemical fuels by splitting water. The only product of using hydrogen gas from water photoelectrolysis is environmental friendly water vapor. Therefore, solar water splitting is an optimal method for solving the energy crisis. Among numerous semiconductor materials, silicon (Si) is the optimal photocathode because of its small band gap and negative conduction band edge. Consequently, Si photocathode absorbs the visible light of solar spectrum and drives solar hydrogen evolution reaction. However, the low kinetics of photo-induced carriers in Si photocathode restricted its photoelectrochemical performance. Moreover, the formation of an insulating oxidation layer on Si photocathode during the exposure of aqueous electrolyte contributed to its photocatalytic degradation or deactivation. In the present study, three dominant strategies were developed to improve the performance and durability of Si photocathode. Surface plasmon resonance metal particles and co-catalyst material modification were applied to enhance the efficiency of the Si photocathode. A passivation layer served as a protective shell that is attached to the Si photocathode to increase its stability. | en |
dc.description.provenance | Made available in DSpace on 2021-06-15T13:08:19Z (GMT). No. of bitstreams: 1 ntu-105-D01223109-1.pdf: 13061316 bytes, checksum: b070e049a3c2138c137f8538451fd6ac (MD5) Previous issue date: 2016 | en |
dc.description.tableofcontents | 口試委員會審定書.....i
誌謝.....ii 摘要.....iii Abstract.....iv Content.....v Figure Caption.....x Table Caption.....xxiv Chapter 1. Introduction.....1 1.1 Solar Water Splitting.....2 1.1.1 History of Solar Water Splitting.....2 1.1.2 Criteria of Solar Water Splitting.....4 1.2 Si-based Photoelectrode.....6 1.2.1 Si Microwire Array Photoelectrode.....8 1.2.2 Metal-assisted Chemical Etching.....10 1.2.3 Plasmon Etching.....12 1.2.4 Vapor–Liquid–Solid Growth.....14 1.3 Strategies for Performance Improvement of Si-based Photoelectrode.....16 1.3.1 Co-catalyst Decoration.....16 1.3.2 Heterojunction Modification.....23 1.3.3 Plasmon Enhancement.....26 1.3.4 Passivation Layer Stabilization.....30 1.4 Research Motivation.....34 References (Chapter 1).....36 Chapter 2. Photoelectrode Materials Preparation and Characterization Techniques.....43 2.1 Chemicals.....44 2.2 Preparation of Photoelectrode Materials.....46 2.2.1 Fabrication of Si Microwire Arrays.....46 2.2.2 Fabrication of Ag-Si Microflower Arrays.....47 2.2.3 Fabrication of Ag-Si Microwire Arrays.....48 2.2.4 Fabrication of Pt-Si Microwire Arrays.....48 2.2.5 Fabrication of Marcasite CoSe2-Si Microwire Arrays.....49 2.2.6 Fabrication of Marcasite CoSe2/C3N4-Si Microwire Arrays.....51 2.2.7 Fabrication of Pyrite CoS2-Si Microwire Arrays.....52 2.2.8 Fabrication of Pyrite CoSe2-Si Microwire Arrays.....54 2.2.9 Fabrication of Si@MoS2 and Si@MMoSx Microwire Arrays.....55 2.3 Photoelectrochemical Water Splitting Measurement.....58 2.3.1 Photoelectrochemical Activity Characterization.....58 2.3.2 Incident Photon-to-electron Conversion Efficiency (IPCE).....62 2.3.3 Gas Evolution Characterization.....63 2.3.4 Electrochemical Impedance Spectroscopy (EIS).....65 2.4 Electrochemical Water Splitting Measurement.....67 2.4.1 Electrochemical Activity Characterization.....67 2.4.2 Tafel Plot Characterization.....68 2.4.3 Electrochemical Double-layer Capacitance Characterization.....70 2.5 Instruments for Characterization of Photoelectrode Materials.....72 2.5.1 X-ray Diffraction (XRD).....72 2.5.2 X-ray Photoelectron Spectroscopy (XPS).....75 2.5.3 X-ray Absorption Spectroscopy (XAS).....77 2.5.4 Scanning Electron Microscopy (SEM).....81 References (Chapter 2).....84 Chapter 3. Ag-Si Microwires Photocathode for Plasmon-enhanced Solar Water Splitting.....85 3.1 Introduction.....85 3.2 Experimental.....88 3.2.1 FEM Simulation of Ag-Si Microwires.....88 3.3 Results and Discussion.....88 3.3.1 Preparation and Chraterization of Ag-Si Microwires.....88 3.3.2 Photoelectrochemical Performance of Ag-Si Microwires.....96 3.4 Summary.....115 References (Chapter 3).....116 Chapter 4. Heterostructure of Si and CoSe2: A Promising Photocathode Based on a Non-noble Catalyst for Photoelectrochemical Hydrogen Evolution.....119 4.1 Introduction.....119 4.2 Experimental.....122 4.2.1 Theoretical Computational Calculation of CoSe2-Si Microwires.....122 4.3 Results and Discussion.....123 4.3.1 Preparation and Chraterization of CoSe2-Si Microwires.....123 4.3.2 Photoelectrochemical Performance of CoSe2-Si Microwires.....131 4.4 Summary.....139 References (Chapter 4).....140 Chapter 5. CoSe2 Grafted in C3N4 function as Efficient Photocathode for Photoelectrochemical Water Splitting.....144 5.1 Introduction.....144 5.2 Results and Discussion.....145 5.2.1 Preparation and Chraterization of Si@CoX2 Microwires.....145 5.2.2 Photoelectrochemical Performance of Si@CoX2 Microwires.....148 5.3 Summary.....159 References (Chapter 5).....160 Chapter 6. Integrated Cobalt Disulfide (CoS2) Co-catalyst Passivation Layer on Silicon Microwires for Photoelectrochemical Hydrogen Evolution.....162 6.1 Introduction.....162 6.2 Experimental.....165 6.2.1 Theoretical Computational Calculation of CoS2-Si Microwires.....165 6.3 Results and Discussion.....166 6.3.1 Preparation and Chraterization of CoS2-Si Microwires.....166 6.3.2 Photoelectrochemical Performance of CoS2-Si Microwires.....178 6.3.3 Photoelectrochemical Durability of CoS2-Si Microwires.....190 6.4 Summary.....199 References (Chapter 6).....200 Chapter 7. Wide Range pH-Tolerable Si@Pyrite Cobalt Dichalcogenide Microwire Arrays Photoelectrode for Solar Hydrogen Evolution.....205 7.1 Introduction.....205 7.2 Results and Discussion.....209 7.2.1 Preparation and Chraterization of Si@CoX2 Microwires.....209 7.2.2 Photoelectrochemical Performance of Si@CoX2 Microwires.....214 7.3 Summary.....230 7.4 Photoelectrochemical Activity Comparison between Marcasite and Pyrite Dichalcogenide Co-catalyst.....232 References (Chapter 7).....234 Chapter 8. Amorphous Heterometal-doped Molybdenum Sulfide Decorated Silicon Microwire Array for Water Photoelectrolysis.....240 8.1 Introduction.....240 8.2.1 Preparation and Chraterization of Si@MoS2 and Si@MMoSx Microwires.....245 8.2.2 Photoelectrochemical Performance of Si@MoS2 and Si@MMoSx Microwires.....250 8.3 Summary.....265 References (Chapter 8).....267 Chapter 9. Concluding Remarks.....274 References (Chapter 9).....282 Publications in Scientific Journals.....286 Patents in Application.....289 Publications as Book Chapters.....290 Publications in Conferences.....291 Honors.....293 Appendix.....294 | |
dc.language.iso | en | |
dc.title | 共催化劑修飾之矽基光電極材料應用於光催化水分解 | zh_TW |
dc.title | Co-catalyst Modified Si-based Photoelectrode Materials for Solar Water Splitting | en |
dc.type | Thesis | |
dc.date.schoolyear | 104-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 鄭淑芬,林麗瓊,吳紀聖,林倫年,董崇禮 | |
dc.subject.keyword | 光催化水分解,共催化劑,矽基光電極, | zh_TW |
dc.subject.keyword | Solar Water Splitting,Co-catalyst,Si-based Photoelectrode, | en |
dc.relation.page | 295 | |
dc.identifier.doi | 10.6342/NTU201600449 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2016-06-30 | |
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 |
文件中的檔案:
檔案 | 大小 | 格式 | |
---|---|---|---|
ntu-105-1.pdf 目前未授權公開取用 | 12.76 MB | Adobe PDF |
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。