Luo Tao, Zhang Ying, Xi Jiafeng, Lu Yuchao, Dong Hai
Key Laboratory for Large-Format Battery Materials and System, Ministry of Education, School of Chemistry & Chemical Engineering, Huazhong University of Science and Technology, Wuhan, China.
Analysis Center of College of Science & Technology, Hebei Agricultural University, Huanghua, China.
Front Chem. 2020 Apr 23;8:319. doi: 10.3389/fchem.2020.00319. eCollection 2020.
Complex mixtures were often observed when we attempted to synthesize 4-thio- and 2,4-dithio-glycoside derivatives by double parallel and double serial inversion, thus leading to no or low yields of target products. The reason was later found to be that many unexpected side products were produced when a nucleophile substituted the leaving group on the substrate containing the thioacetate group. We hypothesized that thioacetyl migration is prone to occur due to the labile thioacetate group even under weak basic conditions caused by the nucleophile, leading to this result. Therefore, we managed to inhibit the generation of thiol groups from thioacetate groups by the addition of an appropriate amount of conjugate acid/anhydride, successfully improving the synthesis of 4-thio- and 2,4-dithio-glycoside derivatives. The target products which were previously difficult to synthesize, were herein obtained in relatively high yields. Finally, 4-deoxy- and 2,4-dideoxy-glycoside derivatives were efficiently synthesized through the removal of thioacetate groups under UV light, starting from 4-thio- and 2,4-dithio-glycoside derivatives.
当我们试图通过双平行和双串联转化来合成4-硫代和2,4-二硫代糖苷衍生物时,经常会观察到复杂的混合物,从而导致目标产物的产率为零或很低。后来发现原因是当亲核试剂取代含有硫代乙酸酯基团的底物上的离去基团时,会产生许多意想不到的副产物。我们推测,即使在亲核试剂引起的弱碱性条件下,由于硫代乙酸酯基团不稳定,硫代乙酰基迁移也容易发生,从而导致了这一结果。因此,我们通过加入适量的共轭酸/酸酐成功抑制了硫代乙酸酯基团生成硫醇基团,提高了4-硫代和2,4-二硫代糖苷衍生物的合成效率。以前难以合成的目标产物在此以相对较高的产率获得。最后,从4-硫代和2,4-二硫代糖苷衍生物出发,通过紫外光照射去除硫代乙酸酯基团,高效合成了4-脱氧和2,4-二脱氧糖苷衍生物。