Chen Bo, Zhang Chan, Niu Libo, Shi Xiaozhen, Zhang Huiling, Lan Xingwang, Bai Guoyi
Key Laboratory of Chemical Biology of Hebei Province, College of Chemistry and Environmental Science, Hebei University, Baoding, Hebei, 071002, P.R. China.
Chemistry. 2018 Mar 7;24(14):3481-3487. doi: 10.1002/chem.201704823. Epub 2018 Jan 8.
Ultrasmall ZnO nanoparticles anchored on N-doped carbon materials with a silica support (ZnO/SiO -NC) were fabricated from chitosan and metal ions by using a one-pot self-assembly strategy and were successfully applied to the synthesis of 2-arylbenzimidazoles under mild conditions. These catalysts showed excellent stability and could be used six times without any loss of conversion and selectivity. The use of silica gel and the biomass chitosan as a source of hydrophilic N-doped carbon materials facilitated the uniform dispersion of the ZnO nanoparticles in methanol and therefore the contact of these nanoparticles with reactants, thus contributing to a high catalytic performance. TEM analysis showed that the ZnO nanoparticles were around 2.55 nm in diameter and uniformly distributed on the support surface. The binding behavior of ZnO and N-doped carbon materials affected the catalytic activity. Interestingly, temperature-programmed NH desorption indicated that the interactions between ZnO and N-doped carbon materials might induce the presence of more acidic sites in these catalysts, thus resulting in enhanced activity and hence promoting this transformation.
通过一锅法自组装策略,以壳聚糖和金属离子为原料制备了负载于二氧化硅载体的氮掺杂碳材料上的超小氧化锌纳米颗粒(ZnO/SiO₂-NC),并成功将其应用于温和条件下2-芳基苯并咪唑的合成。这些催化剂表现出优异的稳定性,可循环使用六次,转化率和选择性均无任何损失。使用硅胶和生物质壳聚糖作为亲水性氮掺杂碳材料的来源,有助于氧化锌纳米颗粒在甲醇中均匀分散,从而使这些纳米颗粒与反应物接触,进而有助于实现高催化性能。透射电子显微镜(TEM)分析表明,氧化锌纳米颗粒的直径约为2.55 nm,均匀分布在载体表面。氧化锌与氮掺杂碳材料的结合行为影响了催化活性。有趣的是,程序升温脱附(NH₃-TPD)表明,氧化锌与氮掺杂碳材料之间的相互作用可能会使这些催化剂中产生更多的酸性位点,从而提高活性并促进这种转化。