氮雜環(huán)雙硫醚配體及二價陽離子模板構筑超分子化合物的合成、結構及光學性能研究
發(fā)布時間:2018-04-25 13:30
本文選題:柔性配體 + 光降解; 參考:《鄭州大學》2017年碩士論文
【摘要】:現(xiàn)階段超分子化學的研究,科學家們已經不再局限于合成具有新穎結構的超分子聚合物,越來越多的研究人員更多關注合成具有特殊功能的超分子聚合物。含氮雜環(huán)有機配體和有機陽離子種類多樣,能夠與Cu/Ag的鹵化物/類鹵化物反應,形成一系列具有結構新穎和獨特的光化學、電化學、磁性、催化及半導體性能的超分子聚合物。本論文合成了四種結構相似的具有不同長度烷基鏈的氮雜環(huán)雙硫醚柔性配體和兩種氮雜環(huán)二價有機陽離子模板,與Cu/Ag的鹵化物/類鹵化物反應,獲得了10個功能性的超分子聚合物,并利用多種表征手段系統(tǒng)研究了化合物1-10的結構和性能。首先我們以4-巰基吡啶為原料合成四個結構相似的柔性雙硫醚配體1,1-二(4-巰基吡啶)甲烷,1,2-二(4-巰基吡啶)乙烷,1,3-二(4-巰基吡啶)丙烷,1,4-二(4-巰基吡啶)丁烷,與Cu/Ag的鹵化物/類鹵化物反應制得化合物1-7,即{[Bpytm]CuI}_n(1),{[Bpyte](CuI_2)_2}n(2),{[Bpytp]Cu I_2}_n(3),{[Bpytp]_3(CuBr_2)_3}_n(4),{[Bpytp]Cu(SCN)_2(CH_3CN)}_n(5),{[Bpytb]Cu(SCN)_2(DMF)}_n(6),{[Bpytb]Ag_2I_3}_n(7)。使用單晶X-射線衍射、紅外光譜、掃描電鏡、能譜分析和元素分析等測試方法對化合物1-7的結構進行了分析,并通過熒光光譜、紫外可見吸收光譜和熱重分析等測試手段對化合物1-7的性質進行了表征。結果表明,化合物1-3為二維網狀結構,化合物4-7為一維鏈狀結構;衔1可作為Fe3+的熒光探針有效檢測Fe3+的存在;在可見光照射下,化合物3-7對有機染料污染物甲基橙(MO)均有較好的降解性能。其次我們以1-乙烯基吡啶、1,3-二(4-氰基吡啶)丙烷為陽離子模板,與CuSCN,CuBr自組裝反應獲得化合物8-10,即{(Pepy)[Cu_2(SCN)_4]}_n(8),{(Pepy)[Cu_2Br_4]}_n(9)和{(Bcpyp)[Cu_2(SCN)_4]}_n(10)。結果表明,化合物8和10都為聚類輪烷結構,分別為二維和三維結構,化合物9呈一維鏈狀結構。在可見光照射下,化合物9-10對有機染料污染物甲基橙(MO)均有較好的降解性能;此外,化合物10在光催化降解羅丹明B(RhB)和亞甲基藍(MB)方面也有顯著的優(yōu)越性。
[Abstract]:At present, the research of supramolecular chemistry is no longer confined to the synthesis of supramolecular polymers with novel structures. More and more researchers pay more attention to the synthesis of supramolecular polymers with special functions. Nitrogen-containing heterocyclic organic ligands and organic cations can react with Cu/Ag halides / halides to form a series of novel and unique supramolecular polymers with novel structure electrochemical magnetic catalytic and semiconductor properties. In this paper, four kinds of flexible ligands with different alkyl chains of different lengths and two bivalent organic cationic templates of heterocyclic nitrogen were synthesized to react with the halides / halides of Cu/Ag. Ten functional supramolecular polymers were obtained and the structures and properties of compounds 1-10 were systematically studied by various characterization methods. Firstly, we synthesized four flexible disulfide ligands (1: 1-1-di- (4-mercaptopyridine)) methane-1 (2)-di- (4-mercapto-pyridine)-ethanethane (1-3-di- 4-mercapto-pyridine) propane with similar structure using 4-mercaptopyridine) as a starting material, and 4---mercapto-pyridine) butane 涓嶤u/Ag鐨勫崵鍖栫墿/綾誨崵鍖栫墿鍙嶅簲鍒跺緱鍖栧悎鐗,
本文編號:1801540
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