請用此 Handle URI 來引用此文件：
http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/100985完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 陳致融 | zh_TW |
| dc.contributor.advisor | Chih-jung Chen | en |
| dc.contributor.author | 林世偉 | zh_TW |
| dc.contributor.author | Shih-Wei Lin | en |
| dc.date.accessioned | 2025-11-26T16:21:34Z | - |
| dc.date.available | 2025-11-27 | - |
| dc.date.copyright | 2025-11-26 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2025-10-01 | - |
| dc.identifier.citation | 參考文獻
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/100985 | - |
| dc.description.abstract | 隨著石化工業的日益進步，全球塑膠製品產量亦持續增長，然而，大量塑膠廢棄物對自然環境造成了嚴重威脅，為應對傳統PET寶特瓶對環境的負面影響，近年來的研究逐漸聚焦於以生物質2,5-呋喃二甲酸(2,5-furandicarboxylic acid; FDCA)為原料製備的生物塑料聚呋喃二甲酸乙二酯(Polyethylene furanoate; PEF)，與石化衍生產物聚對苯二甲酸乙二酯(Polyethylene terephthalate; PET)相比，PEF不僅具有更高的機械強度，還可以從可再生資源中提取，因此被視為PET的永續替代品。
電化學催化羥甲基糠醛(5-hydroxymethylfurfural; HMF)氧化生成FDCA被視為最具未來性的永續生產方法，不僅能夠結合可再生能源驅動反應，實現高附加值化學品的綠色轉化，還能通過產氫反應(hydrogen evolution reaction; HER)生成清潔能源氫氣，然而，為提高反應效率，目前研究多於鹼性溶液中進行，然而在該環境下HMF分子可能引發如歧化反應和自聚合反應等副反應，此外，HER過程中陰極對HMF分子所造成之碳損失在現有研究中常被忽視，為解決上述問題，本次研究引入氧化還原儲庫(redox reservoir; RR)概念，通過氫氧化鎳電極實現了HMF氧化反應與HER的高效解耦，憑藉氫氧化鎳電極稍正的形式電位特性，在開路電位下於純水中(無輔助電解質)自發驅動HMF氧化反應，這不僅消除了對產物的後續純化需求，還避免了副反應所造成的碳損失，在高濃度反應物(300 mM)的條件下，實現超越95%的FDCA產率。 臨場X光吸收光譜(in-situ X-ray absorption spectroscopy)說明RR電極中的Ni3+為反應之活性位點，且反應遵循一級動力學，此外，RR電極的靈活性在糠醛(furfural)氧化生成2-糠酸(2-furoic acid)的成功應用中得到了驗證，表明其對各種含醛基或醇基的生物質分子均具有廣泛適用性。 | zh_TW |
| dc.description.abstract | Plastic production has surged with the growth of the petrochemical industry, causing severe environmental issues. To address the impact of polyethylene terephthalate(PET) bottles, bio-based polyethylene furanoate(PEF), made from biomass-derived 2,5-furandicarboxylic acid (FDCA), has emerged as a sustainable alternative with superior strength and renewable sourcing.
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to FDCA represents a sustainable production route, with the green conversion of biomass into high-value chemicals. Simultaneously, the process generates clean hydrogen energy through the hydrogen evolution reaction (HER). However, to achieve high efficiency, most current studies employ alkaline electrolytes, which induce significant side reactions in HMF molecules, such as disproportionation and self-polymerization. Moreover, carbon loss due to cathodic reduction during HER remains an often-overlooked challenge. Our study introduces redox reservoirs (RRs), using nickel hydroxide electrodes to decouple 5-hydroxymethylfurfural oxidation (HMFOR) and HER. The RR electrode, with its positive formal potential, spontaneously drives HMFOR in pure water under open-circuit conditions, eliminating the need for supporting electrolytes and reducing side reactions. This approach achieves over 95% FDCA yield at high reactant concentrations (300 mM) without requiring product purification. In-situ X-ray absorption spectroscopy identified Ni3+ species as active sites for HMFOR, which follows first-order kinetics. The RR system also demonstrated versatility in oxidizing furfural to 2-furoic acid, highlighting its broad applicability. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2025-11-26T16:21:34Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2025-11-26T16:21:34Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 目次
口試委員審定書 I 誌謝 II 摘要 III Abstract IV 目次 V 圖次 VIII 表次 XIV 第一章 緒論 1 1.1海洋塑膠汙染 1 1.2生物塑料 3 1.2.1生物質 3 1.2.2碳循環 7 1.3羥甲基糠醛氧化反應 8 1.3.1熱催化羥甲基糠醛氧化反應 9 1.3.2光催化羥甲基糠醛氧化反應 10 1.3.3電催化羥甲基糠醛氧化反應 11 1.3.3.1羥甲基糠醛氧化副反應 14 1.3.3.2非鹼性溶液羥甲基糠醛氧化反應 16 1.3.3.3傳統電化學槽進行羥甲基糠醛氧化反應 18 1.4解耦電解反應(decoupled electrolysis) 19 1.4.1氧化還原儲庫 20 1.5研究動機 23 第二章 實驗步驟與儀器分析原理 25 2.1使用之藥品清單 25 2.2電化學分析系統 27 2.3氧化還原儲庫工作電極之製備 28 2.3.1 RR電極粉末漿料製備 29 2.4 HMFOR催化之實驗架設 30 2.4.1高濃度HMFOR催化之實驗架設 30 2.5鈷修飾RR電極置備 31 2.6催化反應之定量分析 32 2.6.1核磁共振光譜儀(Nuclear Magnetic Resonance; NMR) 32 2.6.1.1核磁共振光譜儀原理 32 2.6.1.2核磁共振光譜儀之檢量線建立 33 2.6.2高效液相層析儀(High Performance Liquid Chromatography; HPLC) 35 2.6.2.1高效液相層析儀原理 35 2.6.2.2高效液相層析儀之檢量線建立 37 2.6.3氣相層析儀(Gas Chromatography; GC) 40 2.6.3.1氣相層析儀原理 40 2.6.3.2氣相層析儀之檢量線建立 42 2.7儀器介紹 44 2.7.1 X光繞射儀 (X-Ray Diffraction; XRD) 44 2.7.2 場發射掃描式電子顯微鏡 (Field Emission Scanning Electron Microscope; FE-SEM) 45 2.7.3 X光吸收光譜 (X-ray absorption spectroscopy; XAS) 47 2.7.3.1國家同步輻射研究中心 47 2.7.3.2 X光吸收光譜原理 49 2.7.3.3 X光吸收近邊緣結構(X-ray absorption near-edge structure; XANES) 51 2.8電化學分析原理 53 2.8.1循環伏安法(cyclic voltammetry; CV) 53 2.8.2定電流充放電(Galvanostatic charge/discharge cycle; GCD) 54 第三章 結果與討論 56 3.1氫氧化鎳電極基本鑑定分析 56 3.1.1表面形貌鑑定分析 56 3.1.2晶體結構及組成分析 57 3.2電化學性質量測分析 58 3.2.1氧化還原反應行為及形式電位量測 58 3.2.2解耦效能及電荷儲存能力分析 59 3.3羥甲基糠醛(HMF)化學性質鑑定 62 3.3.1 HMF分子降解分析 62 3.3.2陰極效應 66 3.4 HMFOR催化活性測試 70 3.4.1施加偏壓之催化效能測試 70 3.4.2開路條件之催化效能測試 72 3.5電催化HMFOR之反應機制解析 74 3.5.1 HMFOR產物濃度變化分析 74 3.5.2臨場X光吸收光譜分析 76 3.5.3 HMFOR反應速率解析 79 3.6解耦催化HMFOR及HER之穩定性 88 3.7 RR電極之可調控性 93 3.8 RR電極之催化泛用性 95 第四章 結論 99 參考文獻 100 附錄 112 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 生物質轉換 | - |
| dc.subject | 羥甲基糠醛氧化反應 | - |
| dc.subject | 氧化還原儲庫 | - |
| dc.subject | 解耦催化 | - |
| dc.subject | 無電解質催化反應 | - |
| dc.subject | Biomass Conversion | - |
| dc.subject | 5-Hydroxymethylfurfural Oxidation | - |
| dc.subject | Decoupled Reaction | - |
| dc.subject | Redox Reservoirs | - |
| dc.subject | Electrolyte-Free Reaction | - |
| dc.title | 無電解質自發性之化學生質氧化反應研究 | zh_TW |
| dc.title | Electrolyte-Free Spontaneous Chemical Biomass Oxidation Reaction | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 114-1 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 陳浩銘;陳軍互;盧英睿 | zh_TW |
| dc.contributor.oralexamcommittee | Hao-Ming Chen;Chun-Hu Chen;Ying-Rui Lu | en |
| dc.subject.keyword | 生物質轉換,羥甲基糠醛氧化反應氧化還原儲庫解耦催化無電解質催化反應 | zh_TW |
| dc.subject.keyword | Biomass Conversion,5-Hydroxymethylfurfural OxidationDecoupled ReactionRedox ReservoirsElectrolyte-Free Reaction | en |
| dc.relation.page | 115 | - |
| dc.identifier.doi | 10.6342/NTU202504530 | - |
| dc.rights.note | 同意授權(限校園內公開) | - |
| dc.date.accepted | 2025-10-01 | - |
| dc.contributor.author-college | 重點科技研究學院 | - |
| dc.contributor.author-dept | 奈米工程與科學學位學程 | - |
| dc.date.embargo-lift | 2025-11-27 | - |
| 顯示於系所單位： | 奈米工程與科學學位學程 | |
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