Freedman T B, Ragunathan N, Alexander S
Department of Chemistry, Syracuse University, New York 13244-4100, USA.
Faraday Discuss. 1994(99):131-49; discussion 199-215. doi: 10.1039/fd9949900131.
Vibrational circular dichroism (VCD) spectra in the OH- and NH-stretching regions have been measured for six pharmaceutical molecules in the ephedra class, (1S,2R)-norephedrine, (1), (1S,2S)-norpseudoephedrine (2), (1S,2R)-ephedrine (3), (1S,2S)-pseudoephedrine (4), (1S,2R)-N-methylephedrine (5) and (1S,2S)-N-methylpseudoephedrine (6), all in dilute C2Cl4 solution. Ab initio calculations of geometries and vibrational frequencies for a number of conformers of 1 to 6 have been carried out. The recently developed locally distributed origin gauge model for VCD was used to calculate VCD spectra of the conformers for each drug. This ground-state ab initio model, which does not require sum-over-states, magnetic field perturbation or localized molecular orbitals, has been found to give good agreement with experiment in this frequency region. Composite spectra obtained from weighted averages of the calculated conformer spectra agree within a factor of two with observed IR and VCD intensities for five of the ephedra drugs. For (1S,2S)-pseudoephedrine, the discrepancy between experiment and calculation has been interpreted in terms of a coupled-oscillator effect absent in the other molecules.
已测量了麻黄类六种药物分子,即(1S,2R)-去甲麻黄碱(1)、(1S,2S)-去甲伪麻黄碱(2)、(1S,2R)-麻黄碱(3)、(1S,2S)-伪麻黄碱(4)、(1S,2R)-N-甲基麻黄碱(5)和(1S,2S)-N-甲基伪麻黄碱(6)在稀四氯化碳溶液中的OH和NH伸缩区域的振动圆二色性(VCD)光谱。已对1至6的多个构象异构体进行了几何结构和振动频率的从头算。使用最近开发的VCD局部分布原点规范模型计算了每种药物构象异构体的VCD光谱。已发现这种基态从头算模型,不需要态求和、磁场微扰或定域分子轨道,在该频率区域与实验结果吻合良好。从计算得到的构象异构体光谱的加权平均值获得的复合光谱,与五种麻黄类药物观察到的红外和VCD强度在两倍的范围内相符。对于(1S,2S)-伪麻黄碱,实验与计算之间的差异已根据其他分子中不存在的耦合振子效应来解释。