State Key Laboratory of Elemento-Organic Chemistry, Frontiers Science Center for New Organic Matter, Department of Chemical Biology, College of Chemistry, Nankai University, Tianjin, 300071, China.
Nat Commun. 2023 Sep 1;14(1):5324. doi: 10.1038/s41467-023-41115-x.
In conventional solid-phase peptide synthesis (SPPS), α-amino groups are protected with alkoxycarbonyl groups (e.g., 9-fluorenylmethoxycarbonyl [Fmoc]). However, during SPPS, inherent side reactions of the protected amino acids (e.g., α-C racemization and aspartimide formation) generate by-products that are hard to remove. Herein, we report a thiol-labile amino protecting group for SPPS, the 2,4-dinitro-6-phenyl-benzene sulfenyl (DNPBS) group, which is attached to the α-amino group via a S-N bond and can be quantitatively removed in minutes under nearly neutral conditions (1 M p-toluenethiol/pyridine). The use of DNPBS greatly suppresses the main side reactions observed during conventional SPPS. Although DNPBS SPPS is not as efficient as Fmoc SPPS, especially for synthesis of long peptides, DNPBS and Fmoc are orthogonal protecting groups; and thus DNPBS SPPS and Fmoc SPPS can be combined to synthesize peptides that are otherwise difficult to obtain.
在传统的固相肽合成(SPPS)中,α-氨基用烷氧羰基(例如芴甲氧羰基[Fmoc])保护。然而,在 SPPS 过程中,保护氨基酸的固有副反应(例如,α-C 外消旋化和天冬酰胺亚胺形成)会产生难以去除的副产物。在此,我们报告了一种用于 SPPS 的硫醇不稳定的氨基保护基,即 2,4-二硝基-6-苯基-苯基亚磺酰基(DNPBS)基,它通过 S-N 键连接到α-氨基上,并能在接近中性条件下(1 M 对甲苯硫醇/吡啶)在几分钟内定量去除。DNPBS 的使用极大地抑制了在传统 SPPS 中观察到的主要副反应。虽然 DNPBS SPPS 的效率不如 Fmoc SPPS,尤其是对于长肽的合成,但 DNPBS 和 Fmoc 是正交的保护基;因此,可以将 DNPBS SPPS 和 Fmoc SPPS 结合起来合成其他难以获得的肽。