Kapourani Afroditi, Pantazos Ioannis, Skoutida Stamatia, Assimopoulou Andreana N, Barmpalexis Panagiotis
Laboratory of Pharmaceutical Technology, Division of Pharmaceutical Technology, School of Pharmacy, Faculty of Health Sciences, Aristotle University of Thessaloniki 541 24 Thessaloniki, Greece.
Laboratory of Organic Chemistry, School of Chemical Engineering, Aristotle University of Thessaloniki 54124 Thessaloniki, Greece.
Eur J Pharm Biopharm. 2025 Sep;214:114782. doi: 10.1016/j.ejpb.2025.114782. Epub 2025 Jun 11.
Previous studies have shown that the use of dicarboxylic acid salts can improve the performance of drug amorphous solid dispersions (ASDs), such as in the case of olanzapine (OLN). However, these studies focused only on the use of limited ASD matrices/carriers, e.g. polyvinyl alcohol, overlooking thus the critical impact of their selection on the drug's physical stability and dissolution performance. This study evaluates the performance of ASDs containing fumarate (FUM) and succinate (SUC) drug salts in comparison to ASDs prepared with the drug base, by utilizing the same model drug (i.e., OLN) and various ASD matrices/carriers. Results revealed that inappropriate matrix/carrier selection, even with the more stable amorphous drug salts, led to physical instability (i.e., drug recrystallization) during long term storage. Specifically, only certain matrices/carriers, such as Soluplus® (SOL) for OLN_SUC, copovidone (PVPVA64) or hydroxypropyl cellulose (HPC-SL) for OLN_FUM, and povidone (PVP) for OLN base, were effective in preventing drug recrystallization after three months of storage. Molecular interactions, supported by differential scanning calorimetry (DSC), attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy and molecular dynamics (MD) simulations, demonstrated strong hydrogen bonds between OLN molecules (base and salts) and specific matrices/carriers, contributing to the system's physical stability. Dissolution studies conducted under non-sink conditions further highlighted the importance of matrix/carrier selection for drug supersaturation, with OLN_FUM and OLN_SUC ASDs showing superior performance (higher degree of supersaturation) compared to OLN in its base form. However, all OLN_FUM formulations, as well as OLN_SUC-based ASDs with SOL, showed significant physical instability during solubilization, leading to API's recrystallization in the precipitates collected after dissolution - a pitfall that was not observed in ASD prepared with OLN base and SOL. Hence, the obtained results highlight the necessity of extensive pre-formulation and formulation studies in the preparation of ASDs for various poorly water-soluble drugs (such as OLN) before suggesting dicarboxylate-based drug salts as a one-size-fits-all solution.
先前的研究表明,使用二羧酸盐可以改善药物无定形固体分散体(ASD)的性能,例如奥氮平(OLN)的情况。然而,这些研究仅关注有限的ASD基质/载体的使用,例如聚乙烯醇,因此忽略了它们的选择对药物物理稳定性和溶解性能的关键影响。本研究通过使用相同的模型药物(即OLN)和各种ASD基质/载体,评估含富马酸盐(FUM)和琥珀酸盐(SUC)药物盐的ASD与用药物原料药制备的ASD的性能。结果表明,即使使用更稳定的无定形药物盐,不合适的基质/载体选择也会导致长期储存期间的物理不稳定性(即药物重结晶)。具体而言,只有某些基质/载体,例如用于OLN_SUC的Soluplus®(SOL)、用于OLN_FUM的共聚维酮(PVPVA64)或羟丙基纤维素(HPC-SL)以及用于OLN原料药的聚维酮(PVP),在储存三个月后能有效防止药物重结晶。差示扫描量热法(DSC)、衰减全反射傅里叶变换红外(ATR-FTIR)光谱和分子动力学(MD)模拟支持的分子相互作用表明,OLN分子(原料药和盐)与特定基质/载体之间存在强氢键,有助于系统的物理稳定性。在非漏槽条件下进行的溶出度研究进一步突出了基质/载体选择对药物过饱和的重要性,与原料药形式的OLN相比,OLN_FUM和OLN_SUC ASD表现出优异的性能(更高的过饱和度)。然而,所有OLN_FUM制剂以及基于OLN_SUC且含SOL的ASD在溶解过程中均表现出明显的物理不稳定性,导致在溶解后收集的沉淀物中API重结晶——在用OLN原料药和SOL制备的ASD中未观察到这一缺陷。因此,所得结果突出了在为各种难溶性药物(如OLN)制备ASD时进行广泛的处方前和处方研究的必要性,然后再将基于二羧酸盐的药物盐作为万能解决方案。