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Fatty acid carboxylate-and anionic surfactant-controlled delivery systems that use mesoporous silica supports

机译:使用介孔二氧化硅载体的脂肪酸羧酸盐和阴离子表面活性剂控制的输送系统

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We report the preparation of a MCM-41 mesoporous material that contains the dye [Ru(bipy)_3]Cl_2 (bipy = bipyridine) inside the mesopores and functionalised with suitable binding groups at the entrance of the pores. Solids S1-S3 were obtained by the reaction of the mesoporous material with N-methyl-N'-propyltrimethoxysilylimidazolium chloride, N-phenyl-N-[3- (trimethoxysilyl)propyl]thiourea, or N-phenyl-N'-[3-(trimethoxysilyl)propyl] urea, respectively. A study of the dye delivery of these systems in buffered water (pH 7.0, 2-[4-(2-hydroxyethyl)piperazin-1-yl]ethanesulfonic acid (HEPES), 10~(-3) moldm~(-3)) in the presence of a family of carboxylate ions was carried out. In the interaction of the anions with the surface of the solids, the response depends on the characteristics of the binding groups (i.e., imidazolium, urea and thiourea) at the pore outlets and their specific interaction with the corresponding anion. The interaction of long-chain carboxylate ions with the binding sites at the surface of the solids resulted in a remarkable inhibition of the delivery of the dye. This inhibition was observed clearly for the dodecanoate anion, whereas the octanoate, decanoate, cholate, deoxycholate, glycodeoxycholate and taurocholate anions induced a certain pore blockage that varied according to the solid studied. The interaction of smaller anions, such as acetate, butanoate, hexanoate and octanoate, with the solids had no effect on the dye release process. The possible use of the gating system for the chromo-fluorogenic detection of anionic surfactants through selective dye delivery inhibition was also explored. Molecular dynamic simulations that use force-field methods have been made to theoretically study the capping carboxylate mechanism. The calculations are in agreement with the experimental results, thus allowing a representation of the dye delivery inhibition in the presence of long-chain carboxylate ions.
机译:我们报告了MCM-41中孔材料的制备,该材料在中孔内部包含染料[Ru(bipy)_3] Cl_2(bipy =联吡啶),并在孔的入口处使用合适的结合基团进行了功能化。通过使介孔材料与N-甲基-N'-丙基三甲氧基甲硅烷基咪唑鎓氯化物,N-苯基-N- [3-(三甲氧基甲硅烷基)丙基]硫脲或N-苯基-N'-[3]反应,获得固体S1-S3。 -(三甲氧基甲硅烷基)丙基]脲。这些系统在缓冲水(pH 7.0,2- [4-(2-羟乙基)哌嗪-1-基]乙磺酸(HEPES),10〜(-3)霉菌〜(-3)中的染料输送的研究)在羧酸根离子家族的存在下进行。在阴离子与固体表面的相互作用中,响应取决于孔出口处结合基团(即,咪唑鎓,脲和硫脲)的特性以及它们与相应阴离子的特异性相互作用。长链羧酸根离子与固体表面结合位点的相互作用导致显着抑制染料的传递。十二酸根阴离子可清楚地观察到这种抑制作用,而辛酸根,癸酸根,胆酸根,脱氧胆酸根,糖脱氧胆酸根和牛磺胆酸根阴离子则引起一定的孔堵塞,该孔堵塞因所研究的固体而异。较小的阴离子(例如乙酸根,丁酸根,己酸根和辛酸根)与固体的相互作用对染料释放过程没有影响。还探索了通过选择性抑制染料传递抑制作用,将门控系统用于阴离子表面活性剂的显色荧光检测的可能性。已经进行了使用力场方法的分子动力学模拟,以从理论上研究封端羧酸酯的机理。计算与实验结果一致,因此可以表示在存在长链羧酸根离子的情况下抑制染料传递。

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