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首页> 外文期刊>Chemistry: A European journal >Anions as Triggers in Controlled Release Protocols from Mesoporous Silica Nanoparticles Functionalized with Macrocyclic Copper(II) Complexes
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Anions as Triggers in Controlled Release Protocols from Mesoporous Silica Nanoparticles Functionalized with Macrocyclic Copper(II) Complexes

机译：阴离子作为由大环铜（II）配合物官能化的介孔二氧化硅纳米粒子的控制释放协议中的触发因素

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摘要

Three different mesoporous silica nano-sized materials (SC1, SC2, and SC3), loaded with [Ru(bipy)(3)](2+) dye (bipy= bipyridine) and functionalized on the external surface with three macrocyclic copper(II) complexes (C1, C2, and C3), were synthesized and characterized. When SC1, SC2, and SC3 were suspended in water, the entrapped [Ru(bipy)(3)](2+) dye was free to diffuse from the inner pores to the solution. However, addition of anions induced certain degrees of pore blockage, with subsequent dye release inhibition. Small monovalent and divalent anions were unable to induce complete pore blockage, whereas bulky and highly charged anions induced marked reductions in [Ru(bipy)(3)](2+) delivery. The best [Ru(bipy)(3)](2+) delivery inhibitors were ATP and hexametaphosphate anions. Inhibition was ascribed to the interaction of the anions with the grafted Cu-II complexes on the surface of the SC1, SC2, and SC3 supports. The hexametaphosphate anion was selected to prepare two capped materials (SC1-mPh and SC3-mPh). Studies of the [Ru(bipy)(3)](2+) dye release from solids SC1-mPh and SC3-mPh alone and in the presence of a collection of selected anions (HS-, F-, Br-, Cl-, I-, CN-, HPO42-, AcO-, citrate, NO32-, HCO3-, SO42-, and S2O82-), amino acids (alanine and histidine), thiol-containing biomolecules (cysteine, methylcysteine, homocysteine, and glutathione (GSH)), and oxidants (H2O2) were performed. None of the chemicals tested, except hydrogen sulphide, was able to induce remarkable cargo delivery in both solids. The observed dye release was ascribed to a demetalation reaction of the C1 and C3 complexes induced by the hydrogen sulphide anion.
机译：三种不同的介孔二氧化硅纳米级材料（SC1，SC2和SC3），负载有[Ru（bipy）（3）]（2+）染料（bipy =联吡啶），并在外表面上用三个大环铜（II）进行功能化）复合物（C1，C2和C3）已合成并表征。当SC1，SC2和SC3悬浮在水中时，截留的[Ru（bipy）（3）]（2+）染料会从内孔自由扩散到溶液中。但是，添加阴离子会导致一定程度的孔堵塞，并随后抑制染料释放。小的一价和二价阴离子无法诱导完全的孔堵塞，而笨重的高电荷阴离子则导致[Ru（bipy）（3）]（2+）的输送量明显减少。最好的[Ru（bipy）（3）]（2+）传递抑制剂是ATP和六偏磷酸根阴离子。抑制作用归因于阴离子与SC1，SC2和SC3载体表面上的接枝Cu-II络合物的相互作用。选择六偏磷酸根阴离子可制备两种封端材料（SC1-mPh和SC3-mPh）。 [Ru（bipy）（3）]（2+）染料单独从固体SC1-mPh和SC3-mPh中释放的研究，并且存在一组选定的阴离子（HS-，F-，Br-，Cl- ，I-，CN-，HPO42-，AcO-，柠檬酸盐，NO32-，HCO3-，SO42-和S2O82-），氨基酸（丙氨酸和组氨酸），含硫醇的生物分子（半胱氨酸，甲基半胱氨酸，高半胱氨酸和谷胱甘肽） （GSH））和氧化剂（H2O2）进行。除硫化氢外，所有测试的化学品均无法在两种固体中诱导显着的货物输送。观察到的染料释放归因于由硫化氢阴离子引起的C1和C3络合物的脱金属反应。

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