Zhang Yaoyao, Guo Haifeng, Fu Chengpeng, Fang Zhongpu, Xiong Bo, Li Weishuang, Zhu Bojie Li Lei
School of Chemistry and Materials Science, Hubei Engineering University, Xiaogan 432000, China.
School of Chemistry and Materials Science, Hubei Engineering University, Xiaogan 432000, China.
Int J Biol Macromol. 2025 Jun;311(Pt 4):143865. doi: 10.1016/j.ijbiomac.2025.143865. Epub 2025 May 5.
This work constructed chitosan-based core-shell catalytic nanoreactor (CS/NI/SA@Cu(II)) by free radical polymerization of biomass chitosan and temperature sensitive materials. The CS/NI/SA@Cu(II) were characterized by FT-IR, TG, XPS, SEM, TEM, and EDS to prove the formation of the nanoreactor, and the Cu content was obtained by ICP analysis. The TEM indicated that CS/NI/SA-2 presented a hollow core-shell structure with a size of about 100 nm, and the contact angle of CS/NI/SA-2 was 67°. The core-shell nanoreactors were successfully applied to the 1,4-chiral borylation reaction of α,β-unsaturated compounds, and α,β,γ,δ-unsaturated compounds, as well as the 1,6-chiral borylation reaction of methylene benzoquinone compounds in the aqueous phase. All template substrates can obtain up to 90 % yields with 90 % ee values in core-shell nanoreactors and chiral ligand in 12 h. The possible mechanism of catalytic reaction was revealed by calculation and deuteration experiment. Besides, the CS/NI/SA@Cu(II) could be easily recycled and effectively reused. Besides, the CS/NI/SA@Cu(II) could be easily recycled and effectively reused for 6 times. Remarkably, this approach provides the first report of biomass chitosan for an efficient strategy to gain chiral organic boron compounds in high yields and enantioselectivities.
本工作通过生物质壳聚糖与温度敏感材料的自由基聚合反应构建了基于壳聚糖的核壳催化纳米反应器(CS/NI/SA@Cu(II))。采用傅里叶变换红外光谱(FT-IR)、热重分析(TG)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和能谱分析(EDS)对CS/NI/SA@Cu(II)进行表征,以证明纳米反应器的形成,并通过电感耦合等离子体分析(ICP)获得铜含量。透射电子显微镜表明,CS/NI/SA-2呈现出尺寸约为100 nm的中空核壳结构,CS/NI/SA-2的接触角为67°。该核壳纳米反应器成功应用于α,β-不饱和化合物、α,β,γ,δ-不饱和化合物的1,4-手性硼化反应以及亚甲基苯醌化合物在水相中的1,6-手性硼化反应。在核壳纳米反应器和手性配体存在下,所有模板底物在12小时内均可获得高达90%的产率和90%的对映体过量值(ee值)。通过计算和氘代实验揭示了催化反应的可能机理。此外,CS/NI/SA@Cu(II)易于回收且可有效重复使用6次。值得注意的是,该方法首次报道了利用生物质壳聚糖以高效策略高产率和高对映选择性地获得手性有机硼化合物。