Bisio Antonella, Mantegazza Alessandra, Vecchietti Davide, Bensi Donata, Coppa Alessia, Torri Giangiacomo, Bertini Sabrina
Istituto di Ricerche Chimiche e Biochimiche G. Ronzoni, via G. Colombo 81, Milan 20133, Italy.
Laboratori Derivati Organici, via M. Barozzi 4, Milan 20122, Italy.
Molecules. 2015 Mar 19;20(3):5085-98. doi: 10.3390/molecules20035085.
The evaluation of weight average molecular weight (Mw) and molecular weight distribution represents one of the most controversial aspects concerning the characterization of low molecular weight heparins (LMWHs). As the most commonly used method for the measurement of such parameters is high performance size exclusion chromatography (HP-SEC), the soundness of results mainly depends on the appropriate calibration of the chromatographic columns used. With the aim of meeting the requirement of proper Mw standards for LMWHs, in the present work the determination of molecular weight parameters (Mw and Mn) by HP-SEC combined with a triple detector array (TDA) was performed. The HP-SEC/TDA technique permits the evaluation of polymeric samples by exploiting the combined and simultaneous action of three on-line detectors: light scattering detectors (LALLS/RALLS); refractometer and viscometer. Three commercial LMWH samples, enoxaparin, tinzaparin and dalteparin, a γ-ray depolymerized heparin (γ-Hep) and its chromatographic fractions, and a synthetic pentasaccharide were analysed by HP-SEC/TDA. The same samples were analysed also with a conventional HP-SEC method employing refractive index (RI) and UV detectors and two different chromatographic column set, silica gel and polymeric gel columns. In both chromatographic systems, two different calibration curves were built up by using (i) γ-Hep chromatographic fractions and the corresponding Mw parameters obtained via HP-SEC/TDA; (ii) the whole γ-Hep preparation with broad Mw dispersion and the corresponding cumulative distribution function calculated via HP-SEC/TDA. In addition, also a chromatographic column calibration according to European Pharmacopoeia indication was built up. By comparing all the obtained results, some important differences among Mw and size distribution values of the three LMWHs were found with the five different calibration methods and with HP-SEC/TDA method. In particular, the detection of the lower molecular weight components turned out to be the most critical aspect. Whereas HP-SEC/TDA may underestimate species under 2 KDa when present in low concentration, other methods appeared to emphasize their content.
对重均分子量(Mw)和分子量分布的评估是低分子量肝素(LMWHs)特性表征中最具争议的方面之一。由于测量此类参数最常用的方法是高效尺寸排阻色谱法(HP-SEC),结果的可靠性主要取决于所用色谱柱的适当校准。为了满足LMWHs适当Mw标准的要求,在本工作中采用高效尺寸排阻色谱结合三检测器阵列(TDA)进行了分子量参数(Mw和Mn)的测定。HP-SEC/TDA技术通过利用三种在线检测器的联合和同步作用来评估聚合物样品:光散射检测器(LALLS/RALLS)、折射仪和粘度计。通过HP-SEC/TDA分析了三种市售LMWH样品,依诺肝素、替扎肝素和达肝素,一种γ射线解聚肝素(γ-Hep)及其色谱馏分,以及一种合成五糖。还用采用折射率(RI)和紫外检测器以及两种不同色谱柱组(硅胶柱和聚合物凝胶柱)的传统HP-SEC方法对相同样品进行了分析。在这两种色谱系统中,通过使用(i)γ-Hep色谱馏分和通过HP-SEC/TDA获得的相应Mw参数;(ii)具有宽Mw分散度的整个γ-Hep制剂以及通过HP-SEC/TDA计算的相应累积分布函数,建立了两条不同的校准曲线。此外,还根据欧洲药典的指示建立了色谱柱校准。通过比较所有获得的结果,发现使用五种不同校准方法和HP-SEC/TDA方法时,三种LMWHs在Mw和尺寸分布值之间存在一些重要差异。特别是,低分子量组分的检测结果证明是最关键的方面。虽然当低浓度存在时,HP-SEC/TDA可能会低估2 KDa以下的物种,但其他方法似乎会强调它们的含量。