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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 陳竹亭(Jwu-Ting Chen) | |
| dc.contributor.author | Yi-Hsueh Ho | en |
| dc.contributor.author | 何宜學 | zh_TW |
| dc.date.accessioned | 2021-06-16T08:21:06Z | - |
| dc.date.available | 2017-03-18 | |
| dc.date.copyright | 2014-03-18 | |
| dc.date.issued | 2013 | |
| dc.date.submitted | 2014-01-28 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/58588 | - |
| dc.description.abstract | 本篇論文研究成功的合成出具有N8O2 多牙配體配基，此配基具有多種與金屬配位之可能性。在酸性條件下可成功的合成具雙核銅金屬錯化合物，在鹼性條件下可以成功地得到三核銅金屬錯化合物。雙/三核錯化合物間存在著平衡關係，並且可利用酸鹼加以調控。在可見光光譜滴定實驗中，發現到此平衡中間存在著不穩定的中間體，此中間體可利用質譜儀(ESI-MS)，可見光光譜儀(UV-VIS)以及理論計算加以分析，推測其具有四核銅之特徵。
此外，空氣中二氧化碳可介入此平衡反應，並且被加以捕捉，進而得到八核銅金屬錯化合物。以上之錯化合物皆已使用高解析質譜儀，可見光光譜儀，以及紅外線光譜儀等技術完整鑑定。八合核一雙核銅錯化合物更進一步使用X 光繞射分析儀進行結構解析。 利用雙核銅錯化合物當作模板，再加入額外的異金屬，可成功的合成出混金屬錯化合物。儘管缺少了X 光繞射分析鑑定此混金屬錯化合物之結構，仍利用了可見光光譜儀以及TD-DFT 理論計算決定了此錯化合物之結構以及金屬所在位置。 | zh_TW |
| dc.description.abstract | In this work, new N8O2 multidentate ligands are successfully synthesized and characterized. Their major structures contain three potential binding sites for copper(II) ions and the numbers of metal that bearing multidentate ligand are controlled by pH value. The dinuclear copper(II) complex is successfully synthesized and isolated under acidic condition. When additional copper ions and appropriate base are utilized, the dinuclear complex can be turned to the trinuclear complex. Also, dicopper and tricopper compound can easily take up CO2 to form octanuclear carbonato complex under suitable pH condition. These complexes are fully characterized by UV-VIS, HR-ESI mass, and IR spectroscopy. In addition, the dicopper, and octacopper compound are also studied by single-crystal X-ray diffraction analysis.
According to the information of the dicopper complex can be easily synthesized in acidic condition, it makes the possibility for the synthesis of mixed metal complex. The mixed metal complex have been successfully synthesized and characterized. Despite lack of crystal structure, these mixed metal complexes still can be determined their metal location and geometry by using EPR, UV-VIS and DFT calculation. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-16T08:21:06Z (GMT). No. of bitstreams: 1 ntu-102-D97223130-1.pdf: 11829739 bytes, checksum: 173fc4263097128c27b4c47373099a34 (MD5) Previous issue date: 2013 | en |
| dc.description.tableofcontents | CHAPTER 1 General Introduction
1.1 Hypodentate Complexes 1 1.1.1 Hypodentate Aliphatic Amine Ligands 1 1.1.2 Hypodentate Alicyclic Amine Ligands 4 1.2 Multidentate Ligands binding with Copper 6 1.2.1 Particulate Methane Monooxygenase (pMMO) Model Compound with N6O2 Multidentate Ligands 6 1.2.2 Multidentate Ligands binding with tricopper ions 9 1.3 N8O2 Multidentate Ligand Design 11 CHAPTER 2 Synthesis of N8O2 Ligands and Investigation of Copper(II) Complexes Behaviors 2.1 Design and Synthesis of N8O2 Ligands 13 2.2 Investigation of di/tricopper(II) species from electronic spectrum 16 2.2.1 Synthesis and Characterization of Dinuclear Copper(II) Complexes 18 2.2.2 UV-VIS Spectroscopy and Conductivity of Tricopper(II) Complexes 25 2.2.3 Electrochemistry of tricopper(II) complexes 29 2.2.4 Electron Paramagnetic Resonance (EPR) of Tricopper Complexes 31 2.3 Computational Study of LCu3 36 2.3.1 Geometry Optimization of LCu3 and L’Cu3 37 2.3.2 TD-DFT Calculation of LCu3 42 2.4 Titration Study of LCu3 and H2LCu2 49 Summary of Chapter 2 57 CHAPTER 3 Synthesis and Characterization of Mixed Metal Complexes by N8O2 Multidentate Ligand 3.1 Synthesis and Characterization of LZnCu2 Mixed Metal Complexes 60 3.1.1 UV-VIS Spectroscopy of Mixed Metal Complexes 62 3.1.2 UV-VIS Titration Experiment of Mixed Metal Complexes 63 3.2 Computational Study of Mixed Metal Complex of LZnCu2 70 3.2.1 Geometry optimization of LZnCu2 71 3.2.2 TD-DFT Calculation of LZnCu2 74 3.2.3 Molecular Orbital Analysis of LZnCu2 77 3.3 Investigation of the Intermediate from Titration Experiment of H2LCu2 79 3.4 Synthesis and Characterization of LCuNi2 Mixed Metal Complexes 83 3.4.1 Electron Paramagnetic Resonance (EPR) of Mixed Metal Complexes of LCuNi2 87 3.5 Computational Study of LCuNi2 88 3.5.1 TD-DFT Calculation of LCuNi2 90 Summary of Chapter 3 93 CHAPTER 4 CO2 Fixation by Copper(II) Complexes in the Framework of N8O2 Multidendate Ligand 4.1 Synthesis and Characterization of Octanuclear Copper(II) Carbonato Complexes 96 4.2 Magnetic Properties of LCu8 101 4.3 CO2 absorption pathway of LCu3 108 Summary of Chapter 4 117 CONCLUSION 119 EXPERIMENTAL SECTION 121 REFERENCES 133 APPENDIX 143 | |
| dc.language.iso | en | |
| dc.subject | 多牙配基 | zh_TW |
| dc.subject | 二氧化碳 | zh_TW |
| dc.subject | CO2 Fixation | en |
| dc.subject | Hypodentate | en |
| dc.title | N8O2多牙配基合成及其與後過度金屬配位化學之探討 | zh_TW |
| dc.title | Synthesis of N8O2 Multidentate Ligands and Their Coordination Chemistry on Late Transition Metals | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 102-1 | |
| dc.description.degree | 博士 | |
| dc.contributor.oralexamcommittee | 劉緒宗(Shiuh-Tzung Liu),王瑜(Yu Wang),鄭原忠(Yuan-Chung Cheng),小宮三四郎(Sanshiro Komiya) | |
| dc.subject.keyword | 二氧化碳,多牙配基, | zh_TW |
| dc.subject.keyword | CO2 Fixation,Hypodentate, | en |
| dc.relation.page | 171 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2014-01-29 | |
| 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 | |
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