在本論文中我們將用含有柔軟骨架{Cu2(μ-dppm)2}單元(dppm = bis(diphenylphosphino)methane)的金屬起始物(M)和一些簡單的有機配位基(L)進行自組裝反應，在溶液中M和L尋找自組裝的最佳條件，熱力學最穩定狀態，組合成無法事先預期的有趣結構變化。本論文分成兩部分，茲分述如下:

在第一篇中，M=[(Cu2(μ-dppm)2(NCMe)2]X2 (1X2; X- = BF4-、PF6- 或 BPh4-)分別和L=2-PyCO2H、3-PyCO2H、4-PyCO2H，在CH2Cl2溶液一鍋反應自組裝成環狀二聚物[(Cu2(μ-dppm)2(μ-2-PyCO2)]2X2 (2X2)、環狀二聚物 [(Cu2(μ-dppm)2(μ-3-PyCO2)]2X2 (3X2)、環狀四聚物 [(Cu2(μ-dppm)2(μ-4-PyCO2)]4X4 (4X4)。然而，M和L的自組裝，仍然會受限立體阻礙因素，而形成非環狀結構的形成。就像[(Cu2(μ-dppm)2(NCMe)2](BF4)2和L = 6-Me-3-PyCO2H組裝得到未成環的結構[Cu2(μ-dppm)2(μ-6-Me-3-PyCO2)](BF4) (5(BF4))，並用X-ray繞射儀解出以上四者單晶構造。

在第二篇中，根據文獻含雙架橋系統{Cu2(μ-dppm)2}和bpy (4,4’-bipyridine)、bpyen (trans-1,2-bis(4-pyridyl)ethene) 都聯接成無限延伸的聚合物結構。然而，我們將用含三架橋系統的金屬起始物M=[Cu2(μ-dppm)2(μ-RCO2)](BF4) (R = H, CH3, CH2CH2Ph)和雙吡啶直線型配位基L進行自組裝，搭配了IR、NMR、元素分析輔佐，並用X-ray繞射儀解出單晶構造。當L = bpy時，結構較剛硬，兩個吡啶環幾近共平面，受立體因素影響，而形成寡聚物:[{Cu2(μ-dppm)2(μ-HCO2)}2(μ-bpy)](BF4)2 (9(BF4)2)和[{Cu2(μ-dppm)2(μ-OAc)}2(μ-bpy)(k1-bpy)2](BF4)2 (10(BF4)2)；然而，當L = bpye (1,2-bis(4-pyridyl)ethylane)、bpyen (trans-1,2-bis(4-pyridyl)ethylene)、tmbpy (4,4’-trimethylene-dipyridine)時，由於兩個吡啶環間結構柔軟，兩個吡啶環間可稍扭曲，以利形成聚合物: [{Cu2(μ-dppm)2(μ-OAc)}(μ-bpyen)]n(BF4)n (11(BF4)n)、 [{Cu2(μ-dppm)2(μ-OAc)}(μ-tmbpy)]n(BF4)n (12(BF4)n)、[{Cu2(μ-dppm)2(μ-CO2CH2CH2Ph)}(μ-bpyen)]n(BF4)n (13(BF4)n) 、[{Cu2(μ-dppm)2(μ-CO2CH2CH2Ph)}(μ-bpye)]n(BF4)n (14(BF4)n) 。同時，我們也得到X-ray聚合物單晶構造: 13(PF6)n和14(PF6)n，顯然地，固態寡聚物或聚合物單晶構造不受陰離子改變而影響。多樣的結構變化受螯合基(RCO2-)和架橋基(L)的長度、柔軟度和所採的構形影響。並且寡聚物和聚合物的1H和31P{1H} NMR光譜都極為簡單，在溶液間為一簡單快速的平衡態。

We report herein that the self-assembly of metal starting materials (M) containing flexible skeleton units, {Cu2(μ-dppm)2} (dppm = bis(diphenyl- phos-phino)methane), and simple organic ligands (L) produced some unexpected supramolecular structural variations. And this work is divided into following chapters:

In chapter one, the combination of a flexible ligand-capped dinuclear transition-metal acceptor like [Cu2(μ-dppm)2(NCMe)2]X2 (1X2; dppm = Ph2PCH2PPh2; X- = BF4-, PF6-, or BPh4-) with monodentate-bidentate donors like 2-, 3-, and 4-pyridylcarboxylates produced polygonal oligomeric compounds [{Cu2(μ-dppm)2}(μ-2-PyCO2)]2X2 (2X2), [{Cu2(μ-dppm)2} (μ-3-PyCO2)]2X2 (3X2), and [{Cu2(μ-dppm)2}(μ-4-PyCO2)]4X4 (4X4), respectively, as the thermodynamically stable products in one-pot reactions. However, the modified self-assembly is still subject to steric hindrance. The reaction of complex 1(BF4)2 with 6-Me-3-PyCO2H did not produce a polygonal dimeric metallacycle but a simple dinuclear complex, [Cu2(μ- dppm)2(μ-6-Me-3-PyCO2)] (BF4) (5(BF4)). The crystal structures of complexes 2(PF6)2, 3(PF6)2, 4(BF4)4, and 5(BF4) were determined using X-ray diffraction methods.

In capter two, the assemly of triply bridged binuclear precursors M = [Cu2(μ-dppm)2(μ-RCO2)](BF4) (R = H, CH3, CH2CH2Ph)with linear dipyridyl ligands(L) like 4,4’-bipyridine and its derivatives produced into both oligomers and one-dimensional polymers. These new complexes are characterized by elemental analysis, IR, NMR spectra, together with the solid-state structures of 9-14 determined by X-ray diffraction methods. When L = bpy (4,4’-bipyridine), cation fragments form oligomers: [{Cu2(μ-dppm)2(μ-HCO2)}2(μ-bpy)](BF4)2 (9(BF4)2) and [{Cu2(μ-dppm)2(μ-OAc)}2(μ-bpy)(k1-bpy)2](BF4)2 (10(BF4)2). When L = bpye (1,2-bis(4-pyridyl)-ethane), bpyen (trans-1,2-bis(4-pyridyl)ethylene), tmbpy (4,4’-trimethylene-dipyridine), cation fragments form polymers: [{Cu2(μ-dppm)2(μ-OAc)}(μ-bpyen)]n(BF4)n (11(BF4)n), [{Cu2(μ-dppm)2(μ-OAc)}(μ-tmbpy)]n(BF4)n (12(BF4)n), [{Cu2(μ-dppm)2(μ-CO2CH2CH2Ph)}(μ-bpyen)]n(BF4)n (13(BF4)n) and [{Cu2(μ-dppm)2(μ-CO2CH2CH2Ph)}(μ-bpye)]n (BF4)n (14(BF4)n). However, the single crystal evidences (13n+ and 14n+) suggest that structural variations are independent of the used anions (BF4- and PF6-). The structural outcomes in X-ray crystallography may depend on the flexibility and length of the bridging ligands. Besides, the complexes are suggested to exist as an equilibrium mixture of linear oligomeric and polymeric complexes in solution.

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第二篇
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