六元瓜环与配位聚合物[Cd(H_2O)_3Cl(4-PCA)]的超分子自组装及光催化性能
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摘要
本文用水热法合成得到一个六元瓜环(Q[6])与一氯三水(4-吡啶甲酸)合镉(Ⅱ)配位聚合物自组装作用形成的超分子自组装体Q[6]·[Cd(H_2O)_3Cl(4-PCA)]_2·22(H_2O)。自组装体的形成源于瓜环的外壁作用,即Q[6]正电性静电势外壁与配位聚合物中4-吡啶甲酸吡啶环和配位Cl~-离子间的超分子相互作用,以及配位聚合物镉(Ⅱ)离子上配位水分子与瓜环端口羰基氧原子间的氢键作用。该自组装体对溶液中染料具有吸附作用和光催化降解的性能。
In this paper,a supramolecular self-assembly{Q[6]·[Cd(H_2 O)_3Cl(4-PCA) ]_2·22 H_2O} comprising cucurbit[6]uril( Q[6]) and a 4-pyridine carboxylic acid( 4-PCA) and cadmium( Ⅱ) coordination polymer was synthesized with hydrothermal method.The formation of the supramolecular self-assembly was driven by the outer surface interaction of cucurbit[n]uril,which is the supramolecular interactions between positive electro-potential of the outer surface of Q[6]with pyridine ring and Cl-anion in the coordination polymer,and hydrogen bonding interaction between water molecules and the portal carbonyl oxygens atoms of Q[6]. The self-assembly entity has the properties of adsorption and photocatalytic degradation of dyes in solution.
In this paper,a supramolecular self-assembly{Q[6]·[Cd(H_2 O)_3Cl(4-PCA) ]_2·22 H_2O} comprising cucurbit[6]uril( Q[6]) and a 4-pyridine carboxylic acid( 4-PCA) and cadmium( Ⅱ) coordination polymer was synthesized with hydrothermal method.The formation of the supramolecular self-assembly was driven by the outer surface interaction of cucurbit[n]uril,which is the supramolecular interactions between positive electro-potential of the outer surface of Q[6]with pyridine ring and Cl-anion in the coordination polymer,and hydrogen bonding interaction between water molecules and the portal carbonyl oxygens atoms of Q[6]. The self-assembly entity has the properties of adsorption and photocatalytic degradation of dyes in solution.
引文
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[2]Freeman W A,Mock W L,Shih N Y.Cucurbituril[J].J Am Chem Soc,1981,103(24):7367-7368.
[3]Kim J,Jung I S,Kim S Y,et al.New cucurbituril homologues:Syntheses,isolation,characterization,and X-raycrystal structures of cucurbit[n]uril(n=5,7 and 8)[J].JAm Chem Soc,2000,122(3):540-541.
[4]Day A I,Arnold A P,Method for synthesis cucurbiturils[P].WO0068232,2000,8.
[5]Liu J,Lan Y,Yu Z,et al.Cucurbit[n]uril-based microcapsules self-assembled within microfluidic droplets[J].Acc Chem Res,2017,50(2):208-217.
[6]Murray J,Kim K,Ogoshi T,et al.The aqueous supramolecular chemistry of cucurbit[n]urils,pillar[n]arenes and deep-cavity cavitands[J].Chem Soc Rev,2017,46(9):2479-2496.
[7]Ni X L,Xiao X,Cong H,et al.Cucurbit[n]uril-based coordination chemistry:from simple coordination complexes to novel poly-dimensional coordination polymers[J].Chem Soc Rev,2013,42(24):9480-9508.
[8]Ni X L,Xue S F,Tao Zhu,et al.Advances in the lanthanide metallosupramolecular chemistry of the cucurbit[n]urils[J].Coord Chem Rev,2015,287:89-113.
[9]Ni X L,Xiao X,Cong H,et al.Self-assemblies based on the“outer-surface interactions”of cucurbit[n]urils:new opportunities for supramolecular architectures and materials[J].Acc Chem Res,2014,47(4):1386-1395.
[10]Liang L.L,Chen K,Ji N N,et al.Tetrachloride transitionmetal dianion-induced coordination and supramolecular self-assembly of strontium dications to cucurbit[8]uril[J].Cryst Eng Comm,2013,15(13):2416-2421.
[11]Han B X,Wang C Z,Zhao Y,et al.[PMo12O40]3--induced perhydr oxycucurbit[5]uril-based porous supramolecular assemblies[J].Eur J Inorg Chem,2014,(5):831-835.
[12]Kim K.Mechanically interlocked molecules incorporating cucurbituril and their supramolecular assemblies[J].Chem Soc Reviews,2002,31(2):96-107
[13]韩宝航,刘育,葫芦脲.分子识别与组装[J].有机化学,2003,23(2):139-149
[14]Cao M,Lin J X,Lue J,et al.Development of a polyoxometallate-based photocatalyst assembled with cucurbit
[6]uril via hydrogen bonds for azo dyes degradation[J].J Hazard Mat,2011,186(1):948-951.
[15]Han B X,Wang C Z,Chen K,et al.Coordination and supramolecular assemblies of K+/Ln3+to perhydroxycucurbit[5]uril in the presence of[PMo12O40]3-:potential application in isolation of light lanthanides[J].Cryst Eng Comm,2014,16(9):1615-1619.
[16]Wang C Z,Zhao W X,Shen F F,et al.Methyl-substituted cucurbit[6]uril-based microporous supramolecular frameworks for highly selective Et2O/CH3OH adsorption[J].Cryst Eng Comm,2016,18(12),2112-2118.
[17]Yao Y Q,Zhang Y J,Zhang Y Q,et al.Multiple efficient fluorescence emission from cucurbit[10]uril-[Cd4Cl16]8[J].ACS Appl Mater Interfaces,2017,9(46):40760-40765.
[18]Samsonenko D G,Sokolov M N,Virovets A V,et al.Isolation and structural characterization of new indium(III)aqua complexes:trans-[In Cl2(H2O)4]-and trans-[In Cl4(H2O)2]-as supramolecular adducts with Cucurbituril and related studies[J].Eur J Inorg Chem,2001,(1):167-172.
[19]Thuery P,Masc B.Uranyl ion complexation by cucurbiturils in the presence of perrhenic,phosphoric,or polycarboxylic acids.Novel mixed-ligand uranyl-organic Frameworks[J].Crystal Growth&Design,2010,10(2):716-725.
[20]Yang K,Huang Z X,Liu S M,et al.Synthesis and structure of new supramolecular adducts of[PtCl6]2-with Cucurbit[7]urils[J].Wuhan Univ J Nat Sci,2004,9(1):99-101.
[21]林宏艳,林佳凤,田原,等.酰胺基配体构筑的两种铜配合物的组装、结构与催化性能[J].化学研究与应用,2018,30(5):728-735.
[22]林宏艳,田原,曾凌,等.一种多孔三维超分子钴配合物的合成与光催化性能[J].吉林大学学报(理学版),2017,55(1):162-167.