Li Dong, Wang Min, Yang Caiqin, Wang Jing, Ren Guodong
College of Life Sciences, Hebei University, Baoding 071002, China.
Chem Pharm Bull (Tokyo). 2012;60(8):995-1002. doi: 10.1248/cpb.c12-00245.
Azelnidipine, a new dihydropyridine calcium ion antagonist, was protected by patent in Japan. In present study, identifications of the crystal phases, including two polymorphic and a pseudopolymorphic crystal forms of azelnidipine, were attempted using powder X-ray diffraction (PXRD), differential scanning calorimetry (DSC), IR-, Raman-, THz-, and ss-NMR-spectroscopy. PXRD identified three different crystal forms, while, spectroscopy analysis provided the information of crystal structure involving intermolecular interactions. The transition thermodynamics of the azelnidipine polymorphs were extensively investigated by solubility method. The solubility of the two polymorphs of α and β in 50% ethanol at 25, 31, 37, 42, and 49°C was investigated; the values obtained were used to calculate the thermodynamic parameters of the transition reaction. The temperature of polymorphic phase transition in 50% ethanol was 50.78°C, and the values of ΔG(α,β)(θ), ΔH(α,β)(θ), and ΔS(α,β)(θ) at 25°C were -1.18 kJ·mol(-1), -14.81 kJ·mol(-1), and -45.73 J·mol(-1)·K(-1), respectively. Form β was proved to be thermodynamic stable form at room temperature and enantiotropically related with form α. The kinetics of the solid-state decomposition, studied using DSC analysis, showed that the activation energies of decomposition of the polymorphs α and β at high temperatures were 148.67 and 151.93 kJ·mol(-1).
阿折地平是一种新型二氢吡啶类钙离子拮抗剂,在日本获得了专利保护。在本研究中,尝试使用粉末X射线衍射(PXRD)、差示扫描量热法(DSC)、红外光谱、拉曼光谱、太赫兹光谱和固态核磁共振光谱对阿折地平的晶相进行鉴定,包括两种多晶型和一种假多晶型晶体形式。PXRD鉴定出三种不同的晶体形式,而光谱分析提供了涉及分子间相互作用的晶体结构信息。通过溶解度法广泛研究了阿折地平多晶型物的转变热力学。研究了α和β两种多晶型在50%乙醇中在25、31、37、42和49°C下的溶解度;所得值用于计算转变反应的热力学参数。在50%乙醇中多晶型相变的温度为50.78°C,25°C时ΔG(α,β)(θ)、ΔH(α,β)(θ)和ΔS(α,β)(θ)的值分别为-1.18 kJ·mol(-1)、-14.81 kJ·mol(-1)和-45.73 J·mol(-1)·K(-1)。证明β型在室温下是热力学稳定型,且与α型呈对映异构关系。使用DSC分析研究固态分解动力学,结果表明高温下多晶型物α和β的分解活化能分别为148.67和151.93 kJ·mol(-1)。