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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 周必泰(Pi-Tai Chou) | |
dc.contributor.author | Ya-Chien Yu | en |
dc.contributor.author | 余雅倩 | zh_TW |
dc.date.accessioned | 2021-06-08T06:58:28Z | - |
dc.date.copyright | 2009-07-14 | |
dc.date.issued | 2009 | |
dc.date.submitted | 2009-07-07 | |
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Rev. 2005, 249, 545; (f) J. L. C. Rowsell, O. M. Yaghi, Angew. Chem. Int. Ed. 2005, 44, 4670; g) S. Kitagawa, R. Kitaura, S.-i. Noro, Angew. Chem., Int. Ed. 2004, 43, 2334; h) C. N. R. Rao, S. Natarajan, R.Vaidhyanathan, Angew. Chem. Int. Ed. 2004, 43, 1466; i) C. Janiak, Chem. Soc., Dalton Trans. 2003, 2781; j) B. Kesanli, W. Lin, Coord. Chem. Rev. 2003, 246, 305; k) A. Erxleben, Coord. Chem. Rev. 2003, 246, 203; l) S. L. James, Chem. Soc. Rev. 2003, 32, 276. 3.2. (a) J. L. C. Rowsell, A. R. Millward, K. S. Park, O. M. Yaghi, J. Am. Chem. Soc. 2004, 126, 5666; (b) D. N. Dybstev, H. Chun, K. Kim, Angew. Chem. Int. Ed. 2004, 43, 5033; (c) L. Pan, M. B. Sander, X. Huang, J. Li, M. Smith, E. Bittner, B. Bockrath, J. K. Johnson, J. Am. Chem. Soc. 2004, 126, 1308; d) X. Zhao, B. Xiao, A. J. Fletcher, K. M. Thomas, D. Bradshaw, M. J. Rosseinsky, Science 2004, 306, 1012; (e) B. Chen, N.W. Ockwig, A. R. Millward, D. S. Contreras, O. M. Yaghi, Angew. Chem. Int. Ed. 2005, 44, 4745; f) R. E. Morris, P. S. Wheatley, Angew. Chem. Int. Ed. 2008, 47, 4966. 3.3. (a) O. M. Yaghi, C. E. Davis, G. Li, H. Li, J. Am. Chem. Soc. 1997, 119, 2861; (b) H. J. Choi, T. S. Lee, M. P. Suh, Angew. Chem. Int. Ed. 1999, 38, 1405; (c) R. Kitaura, K. Fujimoto, S. Noro, M. Kondo, S. Kitagawa, Angew. Chem. Int. Ed. 2002, 41, 133; (d) T. K. Maji, K. Uemura, H.-C. Chang, R. Matsuda, S. Kitagawa, Angew. Chem. Int. Ed. 2004, 43, 3269; (e) E. Y. Lee, M. P. Suh, Angew. Chem. Int. Ed. 2004, 43, 2798;( f) D. Tanaka, K. Nakagawa, M. Higuchi, S. Horike, Y. Kubota, T. C. Kobayashi, M. Takata, S. Kitagawa, Angew. Chem. Int. Ed. 2008, 47, 3914; g) S. K. Ghosh, S. Bureekaew, S. Kitagawa, Angew. Chem. Int. Ed. 2008, 47, 3403. 3.4. H. K. Chae, D. Y. Siberio-Perez, J. Kim, Y. Go, M. Eddaoudi, A. J. Matzger, M. O’Keeffe, O. M. Yaghi, Nature 2004, 427, 523. 3.5. P. Sozzani, S. Bracco, A. Comotti, L. Ferretti, R. Simonutti, Angew.Chem. Int. Ed. 2005, 44, 1816. 3.6. T. K. Prasad, M. V. Rajasekharan, Cryst. Growth Des. 2006, 6, 488. 3.7. a) L. R. MacGillivray, J. L. Atwood, J. Am. Chem. Soc. 1997, 119, 2592; b) S. K. Ghosh, P. K. Bharadwaj, Inorg. Chem. 2005, 44, 5553. 3.8. R. J. Doedens, E. Yphannes, M. I. Khan, Chem. Commun., 2002, 62. 3.9. a) J. L. Atwood, L. J. Barbour, T. J. Ness, C. L. Raston, P. L. Raston, J. Am. Chem. Soc. 2001, 123, 7192; (b) W. B. Blanton, S. W. Gordon-Wylie, G. R. Clark, K. D. Jordan, J. T. Wood, U. Geiser, T. J. Collins, J. Am. Chem. Soc. 1999, 121, 3551. 3.10. L. J. Barbour, G. W. Orr, J. L. Atwood, Nature, 1998, 393, 671. 3.11. (a) B. Sreenivasulu, J. J. Vittal, Angew. Chem. Int. Ed. 2004, 43, 5769; (b) S. Neogi, P. K. Bharadwaj, Inorg. Chem. 2005, 44, 816; (c) D. L. Reger, R. F. Semeniuc, C. Pettinari, F. Luna-Giles, M. D. Smith, Cryst. Growth Des. 2006, 6, 1068; (d) J. Y. Wu, J. F. Yin, T. W. Tseng, K. L. Lu, Inorg. Chem. Commun., 2008, 11, 314. 3.12. (a) C. Janiak, T. G. Scharman, J. Am. Chem. Soc. 2002, 124, 14010; (b) K. Raghuraman, K. K. Katti, L. J. Barbour, N. Pillarsetty, C. L. Barnes, K. V. Katti, J. Am. Chem. Soc. 2003, 125, 6955; c) B. Q. Ma, H. L. Sun, S. Gao, Angew. Chem. Int. Ed. 2004, 43, 1374. 3.13. Crystal data for 1: C20H24N2O8Zn, Mr = 485.78, monoclinic, space group C 2/c, a = 20.661(1), b = 9.4792(5), c = 22.127(1) A, β = 103.703(1)°, V = 4210.1(4) A3 , Z = 8, μ = 1.217 mm-1, ρcalcd = 1.533 gcm-3, λ (MoKα) = 0.71073 A, GOF = 1.023, R1 (wR2) = 0.0365 (0.0967) [4185 observed (I >2σ(I))] for 4842 (Rint = 0.0207) independent reflections out of a total of 15992 reflections with 280 parameters. Crystal data for 2: C20H18N2O5Zn, Mr = 431.73, triclinic, space group P -1, a = 8.4881(5), b = 10.1176(6), c = 12.7767(8) A, α = 96.930(1)° β = 109.038(1)°, γ = 102.648(2)°, V = 989.9(1) A3 , Z= 2, μ = 1.273 mm-1, ρcalcd = 1.402 gcm-3, λ(MoKα) = 0.71073 A, GOF= 1.036, R1 (wR2) = 0.0461 (0.1004) [3653 observed (I >2σ(I))] for 4530 (Rint = 0.0439) independent reflections out of a total of 12917 reflections with 284 parameters. Data collection was performed on a Bruker SMART ApexCCD diffractometer with graphitemonochromated MoKa radiation. The structures were solved by direct methods by using SHELXTL program and extended by using Fourier techniques. CCDC- (1) and (2) contains the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/conts/retrieving.html 3.14. F.H. Allen, Acta Crystallogr. Sect., 2002, B58, 380. 3.15 (a) M. Mascal, L. Infantes, J. Chisholm, Angew. Chem., Int. Ed. 2006, 45, 32; (b) L. Infantes, S. Motherwell, CrystEngComm., 2002, 4, 454; (c) L. Infantes, J. Chisholm, S. Motherwell, CrystEngComm, 2003, 5, 480. 3.16. A. L. Spek. J. Appl. Cryst., 2003, 36, 7. 3.17. F. Rouquerol, J. Rouquerol, K. Sing, Adsorption by Powders and Porous Solids; Academic Press: London, 1999. 3.18. K. S. W. Sing, Pure Appl. Chem., 1982, 54, 2201. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/26010 | - |
dc.description.abstract | 金屬有機骨架材料(簡稱MOFs)在近年來有顯著的發展,以金屬當中心,然後用共價鍵連接有機配位基團 (主要是O-linker 、N-linker),空間上可無限延伸到1維、二維、三維,不同維度下又可產生多樣的結構,藉由分子內及分子間不同的交互作用改變分子骨架。利用晶體工程 (crystal engineering),在奈米維度下運用多樣的連接器(connector)和鍵結 (linkers)建構出不一樣孔洞材料的骨架。孔洞材料的特性可應用在不同的應用下,例如:小分子的儲備、交換,以及分離等,晶體上的孔洞結構,使得吸附在孔洞的分子和晶體發生動力學轉換,吸脫附的過程,可能會造成晶體構形上的改變以及物理、化學上的變化。
我們主要利用共軛焦顯微鏡研究單晶的金屬有機骨架材料因結構特異性與受光激發後產生的螢光現象。這三個化合物都是以Zn當中心,選用有機發光團當配位基,由於分子間的弱作用力,π–π 作用力和氫鍵等穩定3D結構。利用XRD和TG測量獲得結構和熱穩定的資訊,分子加熱過後發現螢光效率顯著增加,再者,化合物1有很好的吸水性,其特性有保濕應用的潛力,化合物3因為其配位基含有硫原子,對鉛、汞金屬離子等有較好的鍵結能力,且在有機溶液上,也發現己烷會增加螢光效率,故有應用在檢測器上的潛力。 | zh_TW |
dc.description.abstract | The metal-organic frameworks (MOFs) materials has in recent years advanced extensively, so the materials can afford many and various architectures, which are constructed from a variety of molecular building blocks with different interactions between them. Compounds with backbones constructed from metal ions as connectors and ligands as linkers. Metal–ligand compounds that extend “infinitely” into one, two or three dimensions (1D, 2D or 3D, respectively) via some covalent metal–ligand bondings. Because the porous materials have various properties and potential, contain there are many applications, such as separation, heterogeneous catalysis, and gas storage. The adsorption and desorption of guest molecules onto the solid surface also plays an essential role in determining the properties of porous compounds, for instance photophysics, conformation, and even stability.
Our studying is based on the luminescence using confocal microscope owing to transforming the architectures. Some weaker non-covalent interactions, such as hydrogen bonding or π–π stacking are very important for the packing structures of the one- dimensional chains, two-dimensional nets and three-dimensional frameworks. X-ray powder diffraction (XRPD) and thermogravimetric (TG) measurements are commonly used to analyze the stability of structure. These compounds which we study have specific properties of photoluminescence, the enhancement of quantum efficiency after heating. Compound 1 may thus find their potential application in water sensor. Moreover, the water adsorption property may find their potential application in moisturizing. These results exemplify a unique model that the structural constraints acting on the orientation of water by its surrounding and vice versa can be very significant. Compound 3 has functionalized groups that may have potential on organic solvents and metal ions. We found out that cyclohexane or lead ions exist in the structure, the quantum efficiency of fluorescence will be enhanced. | en |
dc.description.provenance | Made available in DSpace on 2021-06-08T06:58:28Z (GMT). No. of bitstreams: 1 ntu-98-R96223122-1.pdf: 10529762 bytes, checksum: 82918dcb339b69d23b0e82543c4439cd (MD5) Previous issue date: 2009 | en |
dc.description.tableofcontents | 口試委員會書…………………………………………………….............................…… i
謝誌………………………………………………………………............................…… ii 中文摘要…………………………………………………………..........................….... iii 英文摘要…………………………………………………………...........................…… iv Chapter 1. Introduction of metal-organic framework 1.1 Introduction of Metal–Organic Frameworks……….……..…...................…1 1.2 The Properties of Connectors and Linkers………….……................….......4 1.3 Forming various pore structure…………………………….......................….6 1.4 Functions of Metal-Organic Frameworks………………..................…..….10 1.5 Dynamic Frameworks with Nanospace……………………....................….15 1.6 Engineering coordination polymers towards applications...…..............20 1.7 References……………………………………………...……........................…26 Figure 1.1 Schematic representation of the definition of 1D, 2D or 3D coordination polymers……………...................................................................3 Figure 1.2 Schematic representation of a coordination polymer versus other extended metal-ligand structures..................................................................3 Figure 1.3 Classes of porous……………………….......……………….…………..…3 Figure 1.4 Components of metal-organic frameworks have various geometries..............…...................................................................................5 Figure 1.5 Examples of different linkers used in metal-organic framework….5 Figure 1.6 Combinations of various inter- and intra- molecular interactions participating in the construction of a MOFs…………………......................…….7 Figure 1.7 Examples of MOFs with various bonding interactions………………..7 Figure 1.8 Classes of porous structures…………………………………...………...9 Figure 1.9 The other classification of porous compounds as 1st, 2nd, and 3rd generation………………………………………………………............................……9 Figure 1.10 IUPAC classification of gas–solid adsorption isotherms……...…12 Figure 1.11 IUPAC classification of hysteresis loop………………..………….…13 Figure 1.12 Classification of guest-induced structure transformations in MOFs...........................................................................................................18 Figure 1.13 Structures in a bistable state………………………………..………...18 Figure 1.14 Schematic representations of function synthons…………….……19 Figure 1.15 Frequently encountered ligands in different areas of property related work of coordination polymers………………………………..….............20 Figure 1.16 Examples of one-dimensional MOFs with the conductive property (1∞[M(L)(μ-L’)])……………………………………………..............................…….23 Figure 1.17 Luminescence spectra……………………………….........................24 Table 1.1 Classification of pores………………………………………….........……13 Table 1.2 Values of the surface area and pore size and pore volume of stable porous coordination polymers…………………...………...................….……..…15 Table 1.3 Function synthons and modules…………………………......…………19 Chapter 2. Introduction to Confocal Microscopy 2.1 Principle of Confocal Microscopy…………………………….....................…29 2.2 Advantages and Disadvantages of Confocal Microscopy…...........….......37 2.3 Fluorescence Excitation and Emission Fundamentals…….…...................39 2.4 References…………………………………………….…..…........................…..45 Figure 2.1 Airy disc surrounded by much fainter concentric circular rings....30 Figure 2.2 Airy diffraction patterns and limit of resolution……………………..31 Figure 2.3 The Airy disk with increasing numerical aperture…………….…….33 Figure 2.4 Confocal microscope…………..........……………………….......…..…36 Figure 2.5 A illustration of electronic transition…………………………..……...39 Figure 2.6 Franck-Condon energy diagram……………………………...………..41 Table 2.1 Resolution and Numerical Aperture by Objective Correction..........32 Table 2.2 Timescale range for these processes of electronic transitions…....40 Chapter 3. 3D conduit-like MOF with Unique 2D Hydrogen Bonded (H2O)16 Ring and Reversible Moisturization Visualized by Luminescence Changes 3.1 Purpose of the Research…………………………………........................…….46 3.2 Versatile architectures of MOFs…………………………….......................…48 3.3 Discussion of Characteristics of MOFs…………………...................………59 3.4 Synthesis, Design, and Analysis…………………………....................……...74 3.5 Conclusion………………………………………………..….........................…..78 3.6 Reference……………………………………………….........................…..…....79 Figure 3.1 Structures of [Zn(dpe)(BDC)]⋅4H2O (1), [Zn(dpe)(BDC)]⋅H2O (2), and [Zn(4-dpds)(BDC)]·1.5H2O·CH3OH (3)………….……..............................……50 Figure 3.2 The 3D pipe-comb-like MOF of compound 1………….…………....53 Figure 3.3 The (H2O)16 water ring basic building unit of 2D water layer......54 Figure 3.4 View of a 3D single diamondoid framework of compound 2……..55 Figure 3.5 The conformation and distance of metals in compound 3…….....56 Figure 3.6 The schematic diagram of compound 3 with interlaced layer.56-57 Figure 3.7 The TG measurement of compound 1……….…………….……...….64 Figure 3.8 The TG measurement of compound 2………………….….……...….65 Figure 3.9 Adsorption and desorption isotherm of compound 1………...65-66 Figure 3.10 The solid state absorption and single crystal emission spectra of compound 1 and 2……………………………………..........................…...………67 Figure 3.11 Effect of heating/cooling on the emission spectra of compound 1..................................................................................................................67 Figure 3.12 Changes of luminescence appearance for compound 1 with decrease of water content………..................................………………………….68 Figure 3.13 The X-ray Powder diffraction of compound 1……………….….....69 Figure 3.14 The TG measurement of compound 3……………….………..….....69 Figure 3.15 Changes of comportment appearance for compound 3 exposure to heat at 120 ℃ and then cooling to RT……………………................….….….70 Figure 3.16 Adsorption and desorption isotherm of compound 3 obtained of N2 gas at 77 K.…….…………………..….……………………..........................….70 Figure 3.17 Adsorption isotherm of compound 3 obtained of H2 gas.…......71 Figure 3.18 Effect of heating/cooling on the emission spectra of compound 3…..............................................................................................................71 Figure 3.19 Changes of luminescence appearance for compound 3 with decrease of water content from left to right…………………….....…..…..…..…72 Figure 3.20 The emission spectra of compound 3 which was air dried two days after bathed in the hot organic solvent…………..…..…............….………72 Figure 3.21 The emission spectra of compound 3 which was air dried two days after bathed in the different metal ions aqueous solution…........………73 Figure 3.22 From the SEM/EDX, the composed information on compound 3 with Pb2+ ions…………………....................……………………..…………...…….73 Table 3.1 Relevant hydrogen-bonding parameters in compound 1….….….54 Table 3.2 The data of different distances between metals of compound 3..56 Table 3.3 Relevant hydrogen-bonding parameters in compound 3………….57 Table 3.4 Dihedral angles of the R−C=N−N=−R units for 1 and 2…………..57 Table 3.5 Crystal data of single crystal and powder sample for compound 1.................................................................................................................57 Table 3.6 The data of [Zn(4-dpds)(BDC)]∙1.5H2O∙CH3OH (3) from XRD.....59 Table 3.7 Photophysical properties of compound 1 and 2……………………...66 | |
dc.language.iso | en | |
dc.title | 金屬有機骨架材料之單晶結構利用共軛焦顯微鏡在螢光上的研究與應用 | zh_TW |
dc.title | Confocal Luminescence Microscopy of Metal-Organic Framework Single Crystals | en |
dc.type | Thesis | |
dc.date.schoolyear | 97-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 林萬寅(Wann-Yin Lin),何美霖(Mel-Lin Ho) | |
dc.subject.keyword | 金屬有機骨架材料,單晶,共軛焦顯微鏡,檢測器,光激發螢光,螢光, | zh_TW |
dc.subject.keyword | Metal-Organic Framework,Single crystal,Confocal,Sensor,Photoluminescence,Fluorescence, | en |
dc.relation.page | 82 | |
dc.rights.note | 未授權 | |
dc.date.accepted | 2009-07-07 | |
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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