【摘要】 成功制备了一种由内腔、疏水性掺氮碳内层和亲水性二氧化硅外层组成的Janus两亲性碳硅双骨架纳米材料C_xN_y@mSiO₂,并首次将Ni-B合金纳米粒子负载在两亲性碳硅纳米材料上制得Ni-B/C_xN_y@mSiO₂催化剂，并用于松香的水相加氢反应。采用SEM、TEM、N₂吸附-脱附、XRD、XPS等方法对催化剂的结构进行分析与表征，结构分析结果表明：该催化剂具有大比表面积的纳米材料的中空结构，有利于传质和底物富集，内层碳骨架中N原子的掺杂使得附加的金属纳米颗粒得以附着，细小的Ni-B非晶态合金粒子均匀地分散在C_xN_y@mSiO₂中空纳米球及mSiO₂外壳层中，亲水性二氧化硅外壳可以提高催化剂的稳定性和分散性。在水/油两相反应体系中，作为固体发泡剂的两亲性纳米催化剂极大地促进了H₂的溶解及与底物的接触。Ni和B原子之间的协同作用可以显著提高催化活性。因此，Ni-B/C_xN_y@mSiO₂催化剂对松香加氢反应表现出良好的催化活性，其催化活性与贵金属Ru和Pd催化剂基本相当。在160℃、 4.0 MPa、 4 h、水油体积比1∶2和催化剂用量（以松香质量计）10%的条件下，松香的转化率为98.77%,四氢枞酸选择性为23.89%,脱氢枞酸GC含量<1%,达到一级氢化松香的标准。所开发的两亲性Ni-B纳米催化剂表现出较好的稳定性和良好的重复使用性能，重复使用6次时，其催化活性没有明显下降。更多还原

【Abstract】 A kind of Janus amphiphilic carbon silicon double skeleton nanomaterial C_xN_y@mSiO₂ consisting of inner cavity, hydrophobic nitrogen doped carbon inner layer and hydrophilic silicon dioxide outer layer was successfully prepared. Ni-B alloy nanoparticles were loaded on amphiphilic carbon-silicon nanomaterials for the first time to prepare Ni-B/C_xN_y@mSiO₂. The catalyst was also used for the aqueous phase hydrogenation of rosin. The structure of the catalyst was analyzed and characterized by SEM, TEM, N₂ adsorption-desorption, XRD and XPS. The results of structural analysis showed that the catalyst had a hollow structure of nanomaterials with large specific surface area, which was conducive to mass transfer and substrate enrichment. The doping of N atoms in the inner carbon skeleton made the additional metal nanoparticles attached, and the fine Ni-B amorphous alloy particles were uniformly dispersed in the C_xN_y@mSiO₂ hollow nanospheres and mSiO₂ shell layers. The hydrophilic silica shell could improve the stability and dispersion of the catalyst. In the water/oil two-phase reaction system, the amphiphilic nano catalyst as a solid foaming agent greatly promoted the dissolution of H₂ and the contact with the substrate. The synergistic effect between Ni and B atoms could significantly improve the catalytic activity. Therefore, the non noble metal Ni-based nano catalyst showed good catalytic activity for rosin hydrogenation, and its catalytic activity was basically equivalent to those of noble metal Ru and Pd catalysts. Under the conditions of 160 ℃, 4.0 MPa, 4 h, water oil volume ratio of 1 ∶2 and catalyst dosage（based on rosin mass） of 10%, the conversion rate of rosin was 98.77%, the selectivity of tetrahydroabietic acid was 23.89%, and the GC content of dehydroabietic acid was less than 1%, indicating that the product reached the standard of Grade I hydrogenated rosin. The developed amphiphilic Ni-B nano catalyst showed stability and good reusability. When it was reused for 6 times, its catalytic activity did not decrease significantly.更多还原