Nairi Valentina, Medda Luca, Monduzzi Maura, Salis Andrea
Department of Chemical and Geological Sciences, University of Cagliari-CSGI and CNBS, Cittadella Universitaria, S.S. 554 bivio Sestu, 09042 Monserrato, CA, Italy.
Department of Chemical and Geological Sciences, University of Cagliari-CSGI and CNBS, Cittadella Universitaria, S.S. 554 bivio Sestu, 09042 Monserrato, CA, Italy.
J Colloid Interface Sci. 2017 Jul 1;497:217-225. doi: 10.1016/j.jcis.2017.03.021. Epub 2017 Mar 6.
In this work the adsorption and the release of ampicillin - a β-lactam penicillin-like antibiotic - from MCM-41, SBA-15, and (amino functionalized) SBA-15-NH ordered mesoporous silica (OMS) materials were investigated. The silica matrices differ for their pore size (SBA-15 vs. MCM-41) mainly, and also for surface charge (SBA-15 and MCM-41, vs. SBA-15-NH). OMS samples were characterized through small-angle X-rays scattering (SAXS), transmission electron microscopy (TEM), N adsorption-desorption isotherms, Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and potentiometric titrations. The quantification of immobilized and released ampicillin was monitored by mean of UV-Vis spectroscopy. Experimental adsorption isotherms evidenced that ampicillin's loading is not related to the pore size (d) of the adsorbent. Indeed the maximal loadings were 237mg/g for SBA-15 (d=6.5nm), 278mg/g for MCM-41 (d=2.2nm), and 333mg/g for SBA-15-NH (d=5.6nm). Loading seems, instead, to be related to the surface charge density (σ) of the sorbent surface. Indeed, at pH 7.4 ampicillin drug is negatively charged and likely prefers to interact with SBA-15-NH (σ=+0.223Cm) rather than the slightly negatively charged silicas (σ=-0.044Cm and σ=-0.033Cm). Similarly, ampicillin release is affected by interfacial interactions. Indeed, we found a burst release from pure silica samples (SBA-15 and MCM-41), whereas a sustained one from SBA-15-NH sample. We explain this behavior as a result of an attractive interaction between the protonated amino group of SBA-15-NH and the negatively charged carboxylate group of ampicillin. In summary, in order to obtain a sustained drug release, the chemical nature of the matrix's surface plays a role which is more important than its textural features. SBA-15-NH matrix is hence a suitable candidate for local sustained release of antibiotic drugs.
在本研究中,对氨苄西林(一种β-内酰胺类青霉素样抗生素)在MCM-41、SBA-15和(氨基官能化的)SBA-15-NH有序介孔二氧化硅(OMS)材料上的吸附和释放进行了研究。这些二氧化硅基质的主要区别在于孔径(SBA-15与MCM-41),以及表面电荷(SBA-15和MCM-41与SBA-15-NH)。通过小角X射线散射(SAXS)、透射电子显微镜(TEM)、N吸附-脱附等温线、傅里叶变换红外光谱(FTIR)、热重分析(TGA)和电位滴定对OMS样品进行了表征。通过紫外-可见光谱法监测固定化和释放的氨苄西林的定量。实验吸附等温线表明,氨苄西林的负载量与吸附剂的孔径(d)无关。实际上,SBA-15(d = 6.5nm)的最大负载量为237mg/g,MCM-41(d = 2.2nm)为278mg/g,SBA-15-NH(d = 5.6nm)为333mg/g。相反,负载量似乎与吸附剂表面的表面电荷密度(σ)有关。实际上,在pH 7.4时,氨苄西林药物带负电荷,可能更倾向于与SBA-15-NH(σ = +0.223 C/m)相互作用,而不是与带轻微负电荷的二氧化硅(σ = -0.044 C/m和σ = -0.033 C/m)相互作用。同样,氨苄西林的释放也受界面相互作用的影响。实际上,我们发现纯二氧化硅样品(SBA-15和MCM-41)有突发释放,而SBA-15-NH样品有持续释放。我们将这种行为解释为SBA-15-NH的质子化氨基与氨苄西林带负电荷的羧基之间存在吸引相互作用的结果。总之,为了实现药物的持续释放,基质表面的化学性质比其结构特征起更重要的作用。因此,SBA-15-NH基质是抗生素药物局部持续释放的合适候选材料。