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通过点击化学工程制备基于[4+6]-型同手性多孔有机笼的手性固定相,用于正相和反相高效液相色谱中的对映体分离。

Engineering thiol-ene click chemistry for the preparation of a chiral stationary phase based on a [4+6]-type homochiral porous organic cage for enantiomeric separation in normal-phase and reversed-phase high performance liquid chromatography.

机构信息

Department of Chemistry, Yunnan Normal University, Kunming 650500, PR China.

Department of Chemistry, Yunnan Normal University, Kunming 650500, PR China.

出版信息

J Chromatogr A. 2023 Nov 22;1711:464444. doi: 10.1016/j.chroma.2023.464444. Epub 2023 Oct 11.

Abstract

In this study, a new chiral stationary phase (CSP) was fabricated by covalent bonding of a [4+6]-type homochiral porous organic cage (POC) CC19-R onto thiolated silica via a thiol-ene click reaction. The CC19-R was synthesized via Schiff-base reaction between 2-hydroxybenzene-1,3,5-tricarbaldehyde and (1R, 2R)-(-)-1,2-diaminocyclohexane. The enantioseparation capability of the resulting CC19-R-based CSP was systematically evaluated upon separating various chiral compounds or chiral pharmaceuticals in normal phase HPLC (NP-HPLC) and reversed phase HPLC (RP-HPLC), including alcohols, organic acids, ketones, diols, esters, and amines. Fifteen racemates were enantioseparated in NP-HPLC and 11 racemates in RP-HPLC. Some racemates have been well separated, such as 4-chlorobenzhydrol, cetirizine (in the form of dihydrochloride), 1,2-diphenyl-1,2-ethanediol, and 3-(benzyloxy)propane-1,2-diol whose resolution values reached 3.66, 4.23, 6.50, and 3.50, respectively. When compared with a previously reported chiral POC-based column (NC1-R column), eight racemates were not separated on the NC1-R column in NP-HPLC and five racemates were not separated in RP-HPLC, but were well resolved on this column, revealing that the enantioselectivity and separable range of chiral POCs-type columns could be significantly widened using this fabricated CC19-R column. Moreover, the resolution performance of the CC19-R column was also compared with commercial Chiralpak AD-H [CSP: Amylose tris(3,5-dimethylphenylcarbamate)] and Chiralcel OD-H [CSP: Cellulose tris(3,5-dimethylphenylcarbamate)] columns. The column also can separate some racemates that could not be separated or not well be separated by the two commercial columns, showing its good complementarity to the two commercial columns on chiral separation. In addition, the column also had good stability and reproducibility with the relative standard deviation (n = 5) of the retention time and resolution lower than 1.0% and 1.8%, respectively, after it had undergone multiple injections (100, 200, 300, and 400 times). This work indicated that the features of good resolution ability and simple synthesis methods using with this POC-based CSP provided chiral POCs with potential application prospects in HPLC racemic separation.

摘要

在这项研究中,通过硫醇-烯点击反应将[4+6]-型同手性多孔有机笼(POC)CC19-R 通过共价键合到巯基化硅胶上,制备了一种新的手性固定相(CSP)。CC19-R 通过 2-羟基苯-1,3,5-三甲醛与(1R,2R)-(-)-1,2-二氨基环己烷之间的席夫碱反应合成。通过在正相高效液相色谱(NP-HPLC)和反相高效液相色谱(RP-HPLC)中分离各种手性化合物或手性药物,系统地评估了所得基于 CC19-R 的 CSP 的对映体分离能力,包括醇、有机酸、酮、二醇、酯和胺。在 NP-HPLC 中分离了 15 个外消旋体,在 RP-HPLC 中分离了 11 个外消旋体。一些外消旋体得到了很好的分离,例如 4-氯苯甲醇、西替利嗪(二盐酸盐形式)、1,2-二苯基-1,2-乙二醇和 3-(苄氧基)丙烷-1,2-二醇,其分辨率值分别达到 3.66、4.23、6.50 和 3.50。与之前报道的基于手性 POC 的柱(NC1-R 柱)相比,在 NP-HPLC 中,有 8 个外消旋体在 NC1-R 柱上未分离,在 RP-HPLC 中,有 5 个外消旋体未分离,但在该柱上得到了很好的分离,表明通过这种制备的 CC19-R 柱可以显著拓宽手性 POC 型柱的对映选择性和可分离范围。此外,还将 CC19-R 柱的分辨率性能与商业 Chiralpak AD-H [CSP:淀粉三(3,5-二甲基苯基氨基甲酸酯)]和 Chiralcel OD-H [CSP:纤维素三(3,5-二甲基苯基氨基甲酸酯)]柱进行了比较。该柱还可以分离一些用两个商业柱不能分离或不能很好分离的外消旋体,显示出其在手性分离方面与两个商业柱具有良好的互补性。此外,该柱在经过多次进样(100、200、300 和 400 次)后,保留时间和分辨率的相对标准偏差(n=5)分别低于 1.0%和 1.8%,具有良好的稳定性和重现性。这项工作表明,使用这种基于 POC 的 CSP 的良好分辨率能力和简单合成方法的特点为 HPLC 外消旋体分离提供了具有潜在应用前景的手性 POC。

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