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Thermodynamics of antibiotics: natural cyclodextrin inclusion complex formation and covering of nano-metric calcite with these substances
Journal of Thermal Analysis and Calorimetry ( IF 3.0 ) Pub Date : 2020-08-05 , DOI: 10.1007/s10973-020-10048-8
Konrad Szaruga , Maja Fuz , Małgorzata Wszelaka-Rylik , Paweł Gierycz

Isothermal titration calorimetry (ITC) has been used to characterize inclusion complex formation of natural (α-, β-, γ-)cyclodextrins with antibiotics (ampicillin—sodium, penicillin G—sodium, streptomycin sulfate) in aqueous solutions. ITC measurements were taken at 298.15 K on Isothermal Titration Calorimeter Nano ITC. The experimental data were analyzed on the basis of the independent site model. Based on the experimental values of equilibrium constant (K) and enthalpy of complex formation (ΔH), the Gibbs energy of complex formation (ΔG) and the entropy of complex formation (ΔS) have been calculated. The analysis of the obtained inclusion complexes show that independently of the kind of cyclodextrin and antibiotics the obtained equilibrium constants are almost the same, but it is a difference between the changes in enthalpies of complex formation for the investigated systems. The stoichiometry of complexes formed both by ampicillin—sodium and by penicillin G—sodium with all the natural cyclodextrins is the same and equal to 1:1 and the complex formation is entropy driven. Three antibiotics (ampicillin—sodium, penicillin G—sodium and streptomycin sulfate) have been used further for covering of the monodisperse calcium carbonate nanoparticles obtained in the reactor (three-phase reaction) with rotating disks. Three series of experiments have been performed. First was connected with adsorption of the antibiotics on the surface on nano-calcite and two others with intercalation of the drugs into nano-metric CaCO3 structure (aggregates). An intercalation has been performed in two ways: one where the antibiotic was added to the reactor chamber at the beginning of the precipitation reaction and second where it was added just after the end of the reaction. Both pure CaCO3 nanoparticle and antibiotic-coated CaCO3 powders were deeply analyzed by the use of the thermogravimetric and the differential scanning calorimetry method. The performed investigations showed that all the antibiotics used can be both adsorbed and intercalated into the nano-metric CaCO3 obtained in the reactor with rotating disks. The different adsorption obtained by different antibiotics was caused by the different interaction between them and nano-calcite, caused by their different structure. The experimental data have allowed also for distinction between the antibiotics molecules present on calcite surface (adsorption) or antibiotics molecules intercalated into the nano-calcite structure. The conducted research shows that both approaches, i.e., formation of inclusion complexes with natural cyclodextrins and covering (adsorption and intercalation) of nano-metric CaCO3, can be successfully implemented for their pharmaceutical applications.



中文翻译:

抗生素的热力学:天然的环糊精包合物形成并用这些物质覆盖纳米方解石

等温滴定热法(ITC)已用于表征天然(α-,β-,γ-)环糊精与抗生素(氨苄青霉素-钠,青霉素G-钠,硫酸链霉素)的包合物形成。在等温滴定热量计Nano ITC上于298.15 K进行ITC测量。在独立站点模型的基础上分析了实验数据。根据平衡常数(K)和络合物形成焓(ΔH)的实验值,络合物形成的吉布斯能(ΔG)和络合物形成的熵(ΔS))已计算。对所获得的包合物的分析表明,与环糊精和抗生素的种类无关,所获得的平衡常数几乎相同,但是对于所研究的系统,其络合物形成焓的变化之间存在差异。氨苄西林钠和青霉素G钠与所有天然环糊精形成的络合物的化学计量相同且等于1:1,且络合物的形成受熵驱动。三种抗生素(氨苄青霉素钠,青霉素G钠和链霉素硫酸盐)已进一步用于用旋转圆盘覆盖反应器中获得的单分散碳酸钙纳米颗粒(三相反应)。已经进行了三个系列的实验。3结构(聚合)。插层的方法有两种:一种是在沉淀反应开始时将抗生素添加到反应室中,另一种是在反应结束后立即添加抗生素。使用热重和差示扫描量热法对纯CaCO 3纳米颗粒和抗生素包被的CaCO 3粉末进行了深入分析。进行的研究表明,所使用的所有抗生素都可以被吸附和嵌入纳米CaCO 3中用旋转盘在反应器中获得。不同抗生素对纳米方解石结构的不同作用,是由于它们与纳米方解石之间相互作用的不同而引起的。实验数据还允许区分存在于方解石表面(吸附)的抗生素分子或插入纳米方解石结构的抗生素分子。进行的研究表明,两种方法,即与天然环糊精形成包合物和覆盖(吸附和嵌入)纳米级CaCO 3,均可成功用于其药物应用。

更新日期:2020-08-05
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